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Universal quantum control in two-electron spin quantum bits using dynamic nuclear polarization. Sandra Foletti1∗, Hendrik Bluhm1∗ , Diana Mahalu2 , Vladimir Umansky2 & Amir Yacoby1 1 Department of Physics, Harvard University, Cambridge, MA 01238, USA Braun Center for Submicron Research, Department of Condensed Matter Physics, Weizmann Institute of Science, Rehovot 76100, Israel *These authors contributed equally to this work. 2 Achieving universal control and prolonging coherence of quantum bits remain some of the most challenging topics in spin-based quantum computation. Logical quantum bits, constructed out of two or more physical quantum bits, can be designed to prolong coherence by operating in a subspace that is less susceptible to the effects of the environment1 . However, such decoherence free subspace may come at the expense of increased complexity in the control of the qubit. Spin based logical qubits composed of two electron spins in a double quantum dot structure have recently been shown to be dynamically protected against the fluctuating nuclear spin environment through rapid exchange of two electrons. While such exchange operation permits rotations around one axis of the qubit, full universal control of the qubit requires a magnetic field gradient between the two dots to enable rotations around a second axis. Here we demonstrate full quantum control of the two electron logical spin qubit with nanosecond operation times. We have used quantum state tomography to characterize the evolution of the qubit state around a continuously tunable combined axis. The magnetic filed gradient is internally generated using dynamic nuclear polarization of the underlying Ga and As nuclear sublattice. Field gradients of several hundred milliTesla can be sustained for more than 30 minutes and lead to precession frequencies that can exceed 1 GHz. The potential realization of quantum computers has attracted a lot of attention because of their promise to perform certain calculations practically intractable for classical computers2. A variety of possible implementations are currently under investigation, including carbon nanotubes3, nitrogen vacancies4 and flux qubits5. In the present work, the two-level quantum bit (basic element of the quantum computer) is encoded in the spin state of two electrons confined in a double-well potential. This semiconductor-based system has potential for good scalability, manipulations are all electrical and potentially fast enough to enable 104 gate operations within the coherence time (essential for quantum error correction). The phase space of the two-level system is on a one-to-one correspondence with the points on the surface of a three dimensional sphere, the Bloch sphere2 , where the basis states (corresponding to the classical 0 and 1) are represented at the north and south pole (Fig.1g). A generic manipulation of the qubit needed to implement universal gate operations requires the ability to perform rotations around two axes in the Bloch sphere6 (for example the z and x-axis). For two-electron spin qubits, rotations around the z axis correspond to the coherent exchange of two electrons and has been recently demonstrated by Petta et al.7 . Rotations around the second axis occur in the presence of a non-uniform magnetic field within the double-well 1 potential, making the two spins precess at different rates. To this end, we take advantage of the interaction of the electrons with the nuclear field of the Ga and As sublattices of the host material. It has been established though, that the fluctuation of this hyperfine field are also a major source of decoherence8–11 . In this Letter we demonstrate the possibility of building up a gradient in hyperfine fields that significantly exceeds the fluctuations and can be sustained for times longer than 30 min. This is done by employing pumping schemes that transfer spin and thus magnetic moment from the electronic system to the nuclear sublattice. The internally created gradient of nuclear field, in excess of 100 mT, together with the coherent exchange of the two electrons allow us to perform rotations around a variable axis. The coherent manipulation is demonstrated via quantum state tomography measurement, with which the trajectory of the evolution of a state within the Bloch sphere can be reconstructed. The double-well potential in which the electrons are confined is created by applying a negative voltage on metal gates deposited on top of a two dimensional electron gas embedded in a GaAs/AlGaAs heterostructure. The negative potential depletes the region underneath the metal gates creating two isolated puddles of electrons (double quantum dot, Fig.1a). The number of electrons in the dots can be controlled by tuning the potential on the gates. We restrict the occupation of the double quantum dot to two electrons, and describe their spatial separation by the parameter ε: for ε ≫ 0 both electrons are in the right quantum dot, the (0,2) configuration; for ε ≪ 0 one electron occupies each dot, also indicated by (1,1). The dots’ charge configuration can be continuously swept through the intermediate configurations by varying the voltages on the metal gates. In the (0,2) charge configuration √ the only energetically accessible spin configuration is the singlet state S(0, 2) = (↑↓ − ↓↑)/ 2 (the arrows indicate the direction of the electron spin in the left and right dot). As we separate the electrons, the two wavefunctions overlap decreases and four spin configurations become energetically available: the singlet S(1, 1) and three √ triplets T0 = (↑↓ + ↓↑)/ 2, T− =↓↓ and T+ =↑↑ (Fig.1b). We select the states S(1, 1) and T0 , both having a vanishing z component of angular momentum, as qubit basis states and lift the degeneracy with the states T− and T+ by applying an external magnetic field Bext . The Zeeman energy Ez = gµB B (g = −0.4 the g-factor for GaAs, µB Bohr’s magneton) shifts the T+ state to lower energies, creating a crossing point with the singlet (marked by a red circle in Fig.1c) at a value of ε that depends on B = Bext + Bnuc , with Bnuc = (Bnuc,L + Bnuc,R )/2 the average hyperfine field (Bnuc,L (Bnuc,R ) the nuclear field felt by the electron in the left (right) dot, Fig.1b). The rate of coherent exchange of the two electrons (rotation around the z-axis) is controlled by the energy splitting between S(1, 1) and T0 , J(ǫ). The rotation around the x-axis is controlled by the z-component of the difference in local magnetic field ∆Bnuc = Bnuc,L − Bnuc,R , if we z thus p let a state evolve around a combined axis J/2z + gµB Bnuc /2x, the precession frequency is −15 z )2 /h (h = 1 · 10 f = J 2 + (gµB ∆Bnuc µeV /T is Plank’s constant). We present two polarization schemes by which the gradient can be increased to values significantly exceeding fluctuations, both making use of the crossing point between S(1, 1) and T+ . At this point, transitions between the two states are driven by the perpendicular component of ∆Bnuc 12 and accompanied by a spin flip of the nuclei in order to conserve the total angular mo2 Figure 1: Pump and measurement schemes. a, SEM micrograph of a device similar to the one measured. Gates GL and GR control the charge configuration of the two dots, the central gates (Nose and Tail) tune the tunnel barrier transparency between the two dots. The average charge configuration is detected by measuring the conductance (GQP C ) through a capacitively coupled quantum point contact. b, Bnuc,L and Bnuc,R are the local magnetic fields experienced by the electrons in the left and right dot through hyperfine coupling with the Ga and As nuclei. c, Schematic representation of the energy levels at the (0,2)-(1,1) charge transition for finite external magnetic field. The detuning ε from the degeneracy point is controlled via a change of voltage on GL and GR. Two pulse cycle are presented: 1) for nuclear pumping the system is moved to point P where S and T+ are degenerate and can mix 2) for the measurement pulse the system is moved to a very negative detuning where the states S and T0 can mix. d, The measurement pulse scheme e, The S-pumping pulse scheme f, The T+ -pumping pulse scheme all shown as a function of GL and GR. g, Geometrical representation (Bloch sphere) of the two level system (S and T0 ) and the two rotation axes allowing the implementation of universal single qubit gates. 3 mentum. In the newly introduced T+ -pumping scheme, the system is swept slowly into (0, 1) and subsequently reloaded into the (1, 1) charge state (Fig.1f). First the right and then the left electron align with the external field due to large Zeeman energy (≈ 12.5 µeV at 500 mT), which preferentially loads a T+ state. Adiabatically sweeping across the S-T+ transition in 100 ns induces a transition from T+ to S with the transfer of a unit of angular momentum ~ to the nuclei. Alternatively, in the previously used S-pumping scheme13 the system is reset to S(0,2) before the sweep across the S −T+ -transition, where the adiabatic passage guarantees a spin flip-flop in the direction opposite to that of the T + cycle (Fig.1e). The magnitude of the induced gradient can be assessed using a measurement scheme known as T2∗ -pulse7 . This works as follows: after resetting the system into a S(0, 2) state, ε is changed and z set to point S in (1,1) for an evolution time τS . Here ∆Bnuc ≫ J(ε)/gµB drives the mixing between S(1, 1) and T0 and the time evolution of the probability of being in a singlet state oscillates as z p(S) ∝ cos2 (gµB ∆Bnuc ·τS /h). When the system is brought back to point M only transitions from S(1, 1) to S(0, 2) are allowed, while T0 remains blocked in the (1,1) charge configuration. This spin-blockade effect allows to map the spin configuration of the state onto a charge configuration14 , which can be determined with a charge sensor15 . Here the sensor is a quantum point contact (QPC) positioned near one side of the double quantum dot (Fig1a). The conductance of the QPC is very sensitive to nearby electrostatic changes: the addition of an electron to one of the dots results in a detectable change of the conductance. The detector signal, averaged over many T2∗ cycles is proportional to the probability of being in a singlet state. We now show that we can reach a steady state polarisation using either cycle and present evidence that the induced polarisation points in opposite directions for the S and the T+ -pumping cycles. We achieve nuclear steady states by alternating between one of the pumping cycles for a time tpump and a measurement pulse T2∗ for 1 s, with a different τS (0 < τS < 30ns) for each iteration. Each curve in Fig.2a is an average over 30 τS sweeps. An example showing 40 repetitions of τS sweeps for tpump = 60 ms is shown in Fig.2b, where an oscillatory signal with a frequency fluctuating around a steady mean is clearly visible. This observation demonstrates a gradient whose mean is larger than its fluctuations and can be kept constant over at least 40 min. The different values of tpump control the steady state value of the gradient in each dataset z (Fig.2a). We observe that the oscillations vanish (corresponding to a ∆Bnuc fluctuating around 0) at moderate S-pumping rather then tpump = 0. This appears to reflect a small polarization effect from the measurement pulses, that can be compensated with S-pumping (see Supplementary Material). To compare the two pumping cycles, we have taken a measurement alternating between them every 40 τS sweeps (see Fig.2c). The data show that upon changing the pump cycle, the oscillations disappear and then recover after a few minutes in a way that suggests a sign change of the gradient. While determining the magnitude of the gradient with measurements of T2∗ , we can probe the average nuclear field by monitoring the position of the S-T+ transition. This should clarify whether spins are flipped only in one or both dots. Figs. 3a,b show interleaved measurements of the position 4 + a 1.10 s T 0.80 s T+ 0.42 s T+ 0.24 s T+ 0.06 s T+ P S 0.00 s 0.03 s S 0.06 s S 0.09 s S 0.13 s S 0.18 s S 1 0.24 s S 0.42 s S 5 10 τ (ns) S 1 PS b 15 time (min) 0 20 25 30 0 21 42 0.4 0 10 20 30 τ (ns) S c 0 20 time (min) 0.45 s S 40 60 + 0.40 s T 80 0 5 10 τS (ns) 15 20 25 Figure 2: Build-up of a gradient with two different pumping cycles. a, Singlet return probability as a function of separation time τS for different tpump . Each line is an average over the last 30 lines of a measurement as the one shown in b.. b, Singlet return probability as a function of separation time τS changing between 0 and 30 ns. Before each second of measurement (each pixel on the line) we run a pump pulse for tpump = 60 ms. Each line is a repetition of the same measurement z and the whole sequence shows the stability of ∆Bnuc over a time scale of 40 min. c, Crossover between S and T+ -pumping. The intermittance and transient frequency change upon switching the z pump pulse suggests that S- and T+ -pumping produce ∆Bnuc of opposite sign. The plotted data 5 is an average over the last nine of ten repetitions, so that the uppermost lines reflect the transition from T+ - to S-pumping. Bext = 1.5 T for these data sets. of the S–T+ transition16 and the oscillatory S–T0 mixing as a function of tpump using the T+ -pump cycle. A shift of the S–T+ transition to the left corresponds to the build-up of an average field Bnuc oriented opposite to the external magnetic field, consistent with spin flips from down to up in the z nuclear system. Fig.3e shows that at Bext = 500 mT, ∆Bnuc reaches 230 mT while Bnuc is about 130 mT. The ratio of nearly a factor 2 indicates that the nuclei are polarized predominantly in one of the two dots. However, measurements at different Bext show a less pronounced difference, implying some degree of polarization in both dots. Data obtained using the S-pumping cycle (Fig.3e) show a z ∆Bnuc that tends to be slightly smaller than the average field. Note that this analysis may be subject to various systematic errors. An imperfect alignment of the sample with the external magnetic field may lead to orbital effects contributing to the calibration of the position of the S-T+ transition via its dependence on Bext . This calibration may also be affected by a small measurement-induced polarization, either in the calibration data or at the beginning of each measurement. Finally, the z S-T+ transition might also shift in response to ∆Bnuc rather than just Bext + Bnuc , although we z estimate this effect to be negligible at least for small values of ∆Bnuc . For the measurements as in Fig. 3b, we introduced an overshoot towards larger ε before returning to M in the measurement z pulse in order to mitigate a loss of contrast for large ∆Bnuc (see Supplementary Material). z In conjunction with the electrically controllable exchange operation, a controllable ∆Bnuc allows single qubit rotations around an axis that can be tilted to any desired angle between 0 and π/2 away from the x-axes (angle θ in Fig. 4d). We demonstrate and characterize such a rotation using state tomography, consisting of three independent measurements of the probability of being in a |Si ≡ |Zi, in an | ↑↓i ≡ |Xi and in a |Si+i|T0i ≡ |Y i state17 , with pulses shown in Fig. 4a. This allows us to fully reconstruct the state time evolution. For each of the measurements, we first prepare an | ↑↓i by loading a (0,2)S and adiabatically switching off J(ε) in (1, 1). The desired rotation is performed by instantaneously setting J to a finite value for a time τrot . Rapidly returning to S(0, 2) allows to measure p(|Zi) ≡ |hZ|ψi|2, whereas slowly increasing J brings | ↑↓i onto |Si and | ↓↑i onto |T0 i, thus allowing the readout of p(|Xi) ≡ |hX|ψi|2. To obtain p(|Y i) ≡ |(hY |)|ψi|2, J is turned off for a time corresponding to a π/2 rotation around the x-axes before z rapidly returning to M. Results of this procedure for a particular choice of J and ∆Bnuc are shown in Fig. 4c as a function of τrot . For ideal pulses, one would expect p(|Xi) (p(|Zi)) to oscillate sinusoidally between 1 (1/2) and some other value determined by the rotation axis, whereas p(|Y i) should vary symmetrically around 1/2. Deviations from this behavior can be attributed to a finite pulse rise time and high pass filtering of the pulses. The first causes an approximately adiabatic drift of the rotation axis which prevents p(|Si) to return to the starting point, whereas the second leads to slightly different ε-offsets and thus different J(ε) for different pulses, causing a 25 % frequency change. Fits to a model (see Supplementary Material) incorporating these effects and z inhomogeneous broadening due to fluctuations in ∆Bnuc give a good match with the data. In Fig. 4d, the data and fits are displayed in the Bloch sphere representation. We estimate that the errors due to measurement noise, pulse imperfections other than those included in the model, incomplete ensemble averaging over nuclear fluctuations and uncertainties in the QPC conductance calibration (Supplementary Material) are on the order of 0.15 for all three probability measurements. They could be substantially reduced by improving the characteristics of our high frequency setup, such 6 0 a b tpump (s) 0.3 0.6 PS 1 0.7 0.9 0.4 1 ε (mV) c 1 d 0 5 τS (ns) 10 0 5 τS (ns) 10 P S 0.9 0.8 0.7 0.7 −0.2 0 0.2 0.4 ε (mV) 0.6 300 e S 200 (Bznuc,L+Bznuc,R)/2 |∆B | z (Bznuc,L+Bznuc,R)/2 −|∆Bz| 0 B nuc (mT) 100 −100 + T −200 0 0.2 0.4 0.6 0.8 1 tpump (s) Figure 3: Comparison of ∆Bznuc and Bnuc a, Line scans of the position of the S–T+ transition as a function of pump time per 2 s measurement interval for T+ -pumping. b, Singlet return probability versus separation time τS under the same pumping conditions. c, Single line scan from the data in a at tpump = 0.6 s. d, corresponding τS sweep from b. The continuous red line is a sinusoidal fit, the dashed line reconstructs the actual, unaliased time dependence of the singlet probability. e, Bnuc z and ∆Bnuc extracted from fits as shown in c, d for increasing and decreasing tpump for both T + and S-pumping. The shift of the S-T + transition was converted to Bnuc using its measured dependence z on Bext (see supplementary material) 16 , ∆Bnuc was obtained from the fitted oscillation frequency after correcting for the aliasing. The dotted line shows the same data before this correction. Bext = 500 mT for these data sets. 7 that pulse compensation schemes would be simpler and pulse dependant variations of J could be eliminated. The mechanism responsible for the large gradient due to pumping is currently unknown. While the spin from an electron is not necessarily deposited equally in the two dots18, 19 , the known z for both S and T+ -pumping. A possible cause might mechanism cannot explain the large ∆Bnuc be a different relaxation rate in the two dots, for example due to a small difference in size20 . The z relation between our results and those in Ref.16 , where a strong suppression of ∆Bnuc was reported, is currently under investigation. The apparent contradiction with the observation of Reilly et al. that S-pumping becomes ineffective at fields exceeding a few tens of mT might be due to a different coupling between the dots and the electron reservoirs (see Supplementary Material). In the present experiment the inhomogenous dephasing of the precession, associated with z slow fluctuations of ∆Bnuc is in the order of 20 ns. With a faster waveform generator (our is limited to 1 ns steps) more than 10 coherent oscillations could be exploited within this time. Furthermore, z the fluctuations in ∆Bnuc could be eliminated with the implementation of feedback loops that could rapidly adjust the pumping time or the pumping efficiency. Compared to previous reports of gate driven spin manipulation21, 22, our approach has the advantage of much shorter pulse times. This means that if the coherence time at high fields is ≈ 10-100 µs as theoretically predicted23–25 , 104 coherent gate operations are within reach, allowing quantum error correction, essential to perform arbitrary long computation. 1. Taylor, J. M. et al. Fault-tollerant architecture for quantum computation using electrically controlled semiconductor spins. Nature Physics 1, 177 (2005). 2. Nielsen, M. A. & Chuang, I. L. Quantum Computation and Quantum Information (Cambridge University Press, 2000). 3. Mason, N., Biercuk, M. & Marcus, C. Local gate control of a carbon nanotube double quantum dot. Science 303, 655 (2004). 4. Childress, L. et al. Coherent dynamis of coupled electron and nuclear spin qubits in diamons. Science 314, 281 (2006). 5. Majer, J. et al. Coupling superconducting qubits via a cavity bus. Nature 449, 443 (2007). 6. Hanson, R. & Burkard, G. Universal set of quantum gates for double-dot spin qubits with fixed interdot coupling. PRL 98, 050502 (2007). 7. Petta, J. R. et al. Coherent manipulation of coupled electron spins in semiconductor quantum dots. Science 309, 2180 (2005). 8. Khaetskii, A. V., Loss, D. & Glazman, L. Electron spin decoherence in quantum dots due to interaction with nuclei. PRL 88, 186802 (2002). 8 a c 1 p(|↑↓〉) b 0.3 p(|Y〉) 0.8 p(|S〉) 0.2 1 0.8 0.6 0.4 0 c Preparation |S〉 dd |S〉 10 τS (ns) 20 30 e |S〉 X-readout |S〉 |↑↓〉 |↑↓〉 |↓↑〉 θ |−Y〉 |↑↓〉 Y-readout |S〉 |↑↓〉 |T 〉 0 |Y〉 |T 〉 0 Figure 4: State tomography and universal gate. a, Pulse schemes to measure the singlet probability p(|Si) ≡ p(|Zi) , the | ↑↓i probability p(| ↑↓i) ≡ p(|Xi) and the |Si + i|T0 i probability p(|Si + i|T0 i) ≡ p(|Y i) after rotation around a tilted, tunable axis. b, Measurements taken with the X,Z and Y pulses (dots) and fits (line) to a numerical solution of the Schrödinger equation of the S–T0 Hamiltonian incorporating the finite pulse rise time and inhomogeneous broadening due z to fluctuations in ∆Bnuc . c, The preparation of an | ↑↓i state is done by adiabatically turning off J. d, Representation of the measured and fitted trajectory in the Bloch sphere. In order to eliminate phase shifts due to the slightly different frequencies (see text), the time scales for the X-data has been rescaled using spline interpolation so that the expected phase relations are maintained. The blue line is a spline interpolation of the data points in panel b.. e, Visualization of the X and Y-readout schemes on the Bloch sphere. 9 9. Merkulov, I. A., Efros, A. L. & M.Rosen. Electron spin relaxation by nuclei in semiconductor quantum dots. PRB 65, 205309 (2002). 10. Witzel, W. M. & Sarma, S. D. Quantum theory for electron spin decoherence induced by nuclear spin dynamics in semiconductor quantum computer architecture. PRB 74, 035322 (2006). 11. Koppens, F. H. L. et al. Control and detection of singlet-triplet mixing in a random nuclear field. Science 309, 1346 (2005). 12. Taylor, J. M. et al. Relaxation, dephasing, and quantum control of electron spins in double quantum dots. PRB 76, 035315 (2007). 13. Reilly, D. J. et al. Exchange control of nuclear spin diffusion in double quantum dots. 14. Johnson, A. C. et al. Triple-singlet spin relaxation via nuclei in a double quantum dot. Nature 435, 925 (2005). 15. Field, M. et al. Measurements of coulomb blockade with a noninvasive voltage probe. PRL 70, 1311 (1993). 16. Reilly, D. J. et al. Suppressing spin qubit dephasing by nuclear state preparation. Science 321, 817 (2008). 17. Altepeter, J. B., Jeffrey, E. R. & Kwiat, P. Photonic state tomography (2005). 18. Gullans, M. in preparation (2008). 19. Stopa, M. in preparation (2008). 20. de Sousa, R. & Sarma, S. D. Theory of nuclear-induced spectral diffusion: Spin decoherence in phosphorus donors in si and gaas quantum dots. PRB 68, 115322 (2003). 21. Koppens, F. H. L. et al. Driven coherent oscillations of a single electron spin in a quantum dot. Nature 442, 766 (2006). 22. Novack, K. C., Koppens, F. H. L., Nazarov, Y. V. & Vandersypen, L. M. K. Coherent control of a single electron spin with electric fielfds. Science 318, 1430 (2007). 23. Yao, W., Liu, R. B. & Sham, L. J. Theory of electron spin decoherence by interacting nuclear spins in a quantum dot. PRB 74, 195301 (2006). 24. Cywinsky, L., Witzel, W. M. & Sarma, S. D. Electron spin dephasing by hyperfine-mediated interactions in a nuclear spin bath. 25. Coish, W., Fischer, J. & Loss, D. Exponential decay in a spin bath. PRB 77, 125329 (2008). 10 Acknowledgements We are grateful for useful discussions with M.D.Lukin, M.Gullans, M.Stopa, J.J.Krich, B.I.Halperin and C.Barthel. We acknowledge support from (GRANTS...) Competing Interests Correspondence The authors declare that they have no competing financial interests. Correspondence and requests for materials should be addressed to A. Y. (email: [email protected] 11