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Electrically driving nuclear spin qubits with microwave photonic bangap resonators A. J. Sigillito,1,∗ A. M. Tyryshkin,1 T. Schenkel,2 A. A. Houck,1 and S. A. Lyon1 1Department of Electrical Engineering, Princeton University, Princeton, New Jersey 08544, USA 2Accelerator and Fusion Research Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA (Dated: January 25, 2017) The electronic and nuclear spin degrees of freedom for donor impurities in semiconductors form ultra coherent two-level systems that are useful for quantum information applications. Spins natu- rallyhavemagneticdipoles,soalternatingcurrent(AC)magneticfieldsarefrequentlyusedtodrive spin transitions and perform quantum gates. These fields can be difficult to spatially confine to singledonorqubitssoalternativemethodsofcontrolsuchasACelectricfielddrivenspinresonance aredesirable. However,donorspinqubitsdonothaveelectricdipolemomentssothattheycannot normallybedrivenbyelectricfields. Inthisworkwechallengethatnotionbydemonstratinganew, all-electric-field method for controlling neutral 31P and 75As donor nuclear spins in silicon through 7 1 modulation of their donor-bound electrons. This method has major advantages over magnetic field 0 control since electric fields are easy to confine at the nanoscale. This leads to lower power require- 2 ments, higher qubit densities, and faster gate times. We also show that this form of control allows for driving nuclear spin qubits at either their resonance frequency or the first subharmonic of that n frequency, thus reducing device bandwidth requirements. Interestingly, as we relax the bandwidth a requirements, we demonstrate that the computational Hilbert space is expanded to include double J quantum transitions, making it feasible to use all four nuclear spin states to implement nuclear- 3 spin-based qudits in Si:As. Based on these results, one can envision novel high-density, low-power 2 quantum computing architectures using nuclear spins in silicon. ] h p INTRODUCTION up a richer computational manifold and makes it feasi- - ble to implement nuclear spin based qudits using 75As t n donors [10]. EversinceFeynman’sseminalpaperenvisioningquan- a tum computers [1], physicists have dreamt of the ability In recent years, schemes for all-electrical control of u q tosimulatecomplexquantumsystems. Inthe90’s,when donor spin qubits have been proposed [11, 12] but no [ quantum algorithms were discovered that could outper- experimental demonstrations have been reported. Some form their best known classical alternatives [2, 3], the success has been shown in fundamentally different spin 1 v interest in quantum computing redoubled. Soon after, systems including defects in SiC [13], quantum dots [14– 0 it was shown that quantum computers could be realized 16],andsinglemoleculemagnets[9],butthisworkrepre- 5 usingtheelectronicandnuclearspinsofdonorsinsilicon sentsthefirstdemonstrationofelectricallydrivennuclear 6 [4]whichhavelongcoherencetimes[5–8]andareintrinsi- magnetic resonance(EDNMR) for donor spins in silicon. 6 cally compatible with industrial semiconductor process- This material system is particularly attractive since it 0 . ing. Because of their smaller gyromagnetic ratios, nu- already boasts record coherence times [6–8], and atomi- 1 clearspinsaremoredifficulttomanipulatethanelectron callypreciselithographytechniquesthatcantrulybenefit 0 spins and are often considered too slow for quantum in- from electrical control are becoming mature[17, 18]. 7 1 formation processing, but could be suitable as a quan- We find that there are two distinct mechanisms which : tum memory [7]. In this work we demonstrate a new, lead to EDNMR depending on the donor species. 31P v scalablemethodforcontrollingnuclearspinsthatshould donor nuclei are driven through modulation of the elec- i X allowonetoperformrapidmanipulationsofnuclearspins tronic orbital states through the spin-orbit Stark shift r in silicon. Using coplanar photonic bandgap resonators, [19–21]. This tilts the direction of the quantization axis a we drive Rabi oscillations on nuclear spins using exclu- of the electronic spins and induces effective anisotropy sively electric fields by employing the donor-bound elec- in the hyperfine interaction. 75As is subject to the same tronasaquantumtransducer,muchinthespiritofrecent form of control but we find that the 75As Rabi frequen- work with single-molecule magnets [9]. Electric control ciesaretoolargeforthiseffecttoberesponsible. Electric hasmajoradvantagesovermagneticcontrolsinceelectric field modulation of the quadrupolar coupling is likely re- fields are easy to spatially confine at nanometer length sponsible for the EDNMR in 75As. scales. The field confinement leads to lower power re- quirements,higherqubitdensities,andfastergatetimes. We also show here that electric field control allows for EXPERIMENTAL METHODS driving spin qubits at either their resonant frequency or the first subharmonic of that frequency, thus reducing In this work, we make use of the hyperfine interaction device bandwidth requirements. Finally, we show that to read out the nuclear spin state (m ) using the Davies I double quantum transitions can be driven which opens electron-nuclear double resonance (ENDOR) technique 2 [22, 23]. In this measurement, one probes the electron B(cid:126) inthedevicewithoutchanging B(cid:126) ortheensembleof 2 1 spin resonance (ESR) transitions while simultaneously spins probed by the ESR. performing nuclear magnetic resonance. The ESR tran- The resonators used in this work were patterned in sition intensity depends on the nuclear spin state, so by a 50 nm thick Nb film e-beam evaporated on the sur- performingconventionalESRonthedonorelectronspin, face of a C-plane sapphire wafer. The structures were one also obtains m . This technique therefore requires defined using optical lithography and SF plasma etch- I 6 bothmicrowavemagnetic(B(cid:126) )andradiofrequencymag- ing as previously described [29, 30]. These resonators 1 netic (B(cid:126) ) fields. In this study, to electrically probe nu- can be patterned directly on the silicon sample to offer 2 clei, we also require RF electric fields (E(cid:126) ) fields. To enhanced sensitivity, but to ensure that the spin signal 2 maintain a suitable signal-to-noise ratio (SNR), a high only comes from the 1/2 wavelength defect region of the quality factor microwave resonator is used. resonator (and not spins within the Bragg mirrors), the samplewasclippedtothesurfaceoftheresonatorusinga CommercialENDORresonatorsexist,buttheyrequire phosphor bronze spring as shown in Fig. 1(b). This par- large powers (making them incompatible with ultra-low ticular device has five periods of Bragg mirror on either temperature measurements) and are designed to pro- side of the half wavelength defect. Each period consists vide RF magnetic, and not electric fields. This led us of both a high impedance (95 Ω, 4 mm long) and a low to develop superconducting coplanar photonic bandgap impedance (30 Ω, 4 mm long) strip of waveguide. The (PBG) resonators which allow broadband RF and mi- cavity is 6 mm long with a 10 µm wide center pin and crowave transmission above and below a lithographi- gap. TheRFterminationisdefinedbyeitherleavingthe cally defined photonic bandgap [24–27]. A schematic of output port floating, or by shorting it to ground using the device is shown in Fig. 1(a). The bandgap is con- aluminum wirebonds. structed by periodically alternating the impedance of a The device was cooled to 1.9 K in a pumped helium superconducting CPW transmission line to form a one- cryostat equipped with a rotatable sample holder. This dimensionalmicrowaveBragggratingasshownschemat- allows for in-situ alignment of the device with an exter- ically in Fig. 1(a). By incorporating a 1/2 wavelength nally applied magnetic field B(cid:126) [30]. With B = 250 mT defect in the photonic bandgap, the device supports a 0 0 applied in the plane of the Nb, the microwave transmis- resonant mode which can be used for ESR. Equivalently sion spectrum was measured and is plotted in Fig. 1(c). this structure can be thought of as two discrete Bragg The photonic bandgap gives about 80 dB of attenua- mirrorsdefiningtheboundariesofahalfwavelengthcav- tion from 4.5 - 9 GHz and the microwave resonance ap- ity[28]. Thesampleislocatedabovethecavityregionof pears at 7.3 GHz. The resonator is slighly undercoupled thedevice. Thisresonatordesignhasacontinuouscenter and has a temperature-limited quality factor of approxi- conductorwhichisisolatedfromthegroundplaneandal- mately 20000. The spin sensitivity of this resonator was lowsforeasyapplicationofDCvoltageorcurrentbiases. determined to be 5 × 106 spins per shot at 2 K using These devices require only one layer of lithography and phosphorus doped 28Si (800 ppm 29Si). This is on par willbeconvenientforotherareasofquantuminformation withotherplanarresonators[29,30]andcouldbefurther processingandESR.Resonatordesignconsiderationsare improved by incorporating quantum-limited parametric outlined in the Supplementary Information. amplifiers [31, 32]. These resonators have a built-in feature which allows The sample used throughout this work consists of a us to easily select whether electric or magnetic RF fields 2 µm isotopically enriched 28Si epitaxial layer grown on are present in the sample. The RF frequencies used a high resistivity p-type substrate. The epi-layer was in this work have a wavelength that is large compared grown to have 5×1015 31P/cm3 and the sample was ion to the scale of the device and are unperturbed by the implanted with 209Bi and 75As. After implantation, the photonic bandgap (since they lie well below the gap). donors were activated by annealing the sample in a N 2 We can therefore set up RF standing waves by termi- atmosphere at 800◦C for 20 minutes [33]. The simulated nating the transmission line at the output port of the implantation profiles are shown in Fig. 2(a) [34]. Two- device (labeled ”variable termination” in Fig. 1(a)). A pulse Hahn echo measurements were performed at 1.9 high impedance (open) termination is used to enhance K and an echo-detected field swept spectrum is shown E(cid:126) whereas a low impedance (shorted) termination en- in Fig. 2(b), revealing the 31P and 75As hyperfine lines. 2 hances B(cid:126) in the sample. Due to the finite size of the Using pulsed spin counting techniques, we estimate the 2 device, one can never fully suppress the E(cid:126) and B(cid:126) fields 209Biactivationtobeabout50%whereasthe75Asdonors 2 2 but we estimate that the residual undesired field ampli- arefullyactivated. Becausethe209Bisignalisveryweak tudesarereducedbyatleastafactorof50inthesample. (due to low donor activation and a large nuclear spin, Themicrowavemagneticfield,B(cid:126) ,hasawavelengththat 9/2), the ENDOR experiments were only performed on 1 issetbytheλ/2sectionofthedeviceandiswellconfined the 31P and 75As donors. by the two Bragg mirrors. It is unperturbed by the ter- In the presence of B(cid:126) inhomogeneity, one can mea- 1 mination off-chip so that we can select between E(cid:126) and sure entirely different subensembles of spins subject to 2 3 FIG. 2. The sample consists of a 31P doped 28Si epitaxial layerwhichhasbeenimplantedwith209Biand75Asasshown in(a). Anechodetectedfieldsweepspectrumisshownin(b) resolving the two 31P and the four 75As hyperfine lines. The hyperfine lines are labeled by their nuclear spin projections with colors matching the data in Fig. 3. These data were taken at 1.9 K with a resonator frequency of 7.3 GHz. frequenciesinthefollowingexperiments,whichwerethus FIG. 1. (a) Cartoon schematic of a photonic bandgap res- conducted using rectangular pulses. onator. The left port of the device is used for microwave Prior to every experiment, the spins were prepared in excitation and readout and the right port can be terminated thermal equilibrium using a combination of RF and op- to select whether RF electric or magnetic fields are present in the device. An optical micrograph of an actual device is tical pulses as described in [23] since nuclear spin relax- shown in (b) with a silicon sample (bright rectangular fea- ation times are long at these temperatures. ture) mounted using a phosphor bronze clip. The serpentine structuresaboveandbelowthesamplearetheBraggmirrors. Theinsetshowsazoomedinviewofanimpedancestep. The RESULTS microwavetransmissionthroughthisstructureisshownin(c) forthedeviceinamagneticfieldof250mTatatemperature of 1.9 K. The photonic bandgap spans the frequency range Davies ENDOR experiments were first performed us- between4.5GHzand9GHzwithnearlylosslesstransmission ingonlyRFmagneticfields(shorteddevicetermination). below 4 GHz. The resonance appears at 7.3 GHz with a Q The ENDOR spectra for all four of the 75As donor hy- factorof20000. Thelossoutsideofthebandgapisduetothe perfinelinesareplottedinFig.3(b)buttheexperiments coaxial test cables which were not calibrated out. were also performed on the 31P donors as shown in the supplementaryinformation. Onlythemagneticdipoleal- lowed transitions could be resolved in this configuration. different RF electric or magnetic fields by varying the Those are ∆m = 0,∆m = ±1, with m and m being s I s I microwave power[29]. It was therefore important to cal- the electronic and nuclear spin projections, respectively. ibrate B(cid:126)1 before every ENDOR experiment by perform- The device was reconfigured to have E(cid:126)2 fields in the ing two-pulse Hahn echo experiments as a function of sample (open termination) and the measurements were microwave power. The electric and magnetic field dis- repeatedwiththeresultsdisplayedinFig.3(c)(31Pdata tributions are well known[20, 30] and are plotted in the availableinthesupplementaryinformation). Inaddition supplementary information. It has been shown that in- to the allowed ENDOR transitions, several additional homogeneity in B(cid:126)1 can be overcome by using adiabatic transitionsappearedinthe75Asspectraandaredenoted (BIR-WURST) pulses [29]. In the supplementary infor- by the arrows. These very narrow transitions occur at mation we demonstrate that they also overcome E(cid:126) in- exactly half the frequency of forbidden double quantum 2 homogeneity. ThesepulseshapingtechniquesmakePBG transitions (∆m = 0,∆m = 2). The single quantum s I resonators useful for complex ENDOR experiments re- transitionsarepowerbroadenedinthisplot, sincepower quiring high fidelity manipulations. We measure Rabi wasoptimizedforthedoublequantumtransitions. Tran- 4 sitionswerealsoobservedatsubharmonicsoftheallowed perfine tensor, I(cid:126) is the nuclear spin, g is the nuclear n transition frequencies and are shown in Fig. 3(d). g-factor, β is the nuclear magneton, and Qˆ is the nu- n The double quantum transitions do not exist for 31P clear quadrupole coupling tensor. The terms in the spin donors since they have nuclear spin-1/2. EDNMR was Hamiltonian that are sensitive to electric fields are the observed at the fundamental and subharmonic transi- electronic Zeeman (gˆ ), hyperfine (Aˆ), and quadrupolar e tions frequencies for 31P, but it was noticed that 31P (Qˆ) tensors. Because EDNMR is observed for both 75As donors require more RF power than 75As donors. To and 31P (which has no quadrupole moment), we first ne- quantify the difference, two dimensional EDNMR mea- glect quadrupolar effects. surements of the Rabi nutation were conducted on both Both Aˆ and gˆ can be modulated through the hyper- e donors. These experiments used the standard Davies fine and spin-orbit Stark effects, respectively. These ef- ENDOR pulse sequence but varied the RF pulse length fects are quadratic to first order due to inversion sym- andpower. Thedataforthesubharmonictransitionsare metry at the donor site, but linear terms can arise from plotted in Fig. 4 (a-b) and the Rabi data for the funda- strain[35, 36]. We therefore expect to drive transitions mentaltransitionsareshowninthesupplementaryinfor- at both the electric field frequency, f, and f/2 (since mation. Fromthedata,itisclearthatthearsenicdonors sin2(f)∝cos(2f)). Similarsubharmonictransitionshave respondoveranorderofmagnitudemorestronglytothe been observed for electrically driven spin resonance in electric fields (shorter RF pulses are necessary); indicat- quantum dots[15, 37]. Since the fundamental transition ingthatdifferentmechanismsmayberesponsibleforthe (at f) is strain dependent, we will restrict our discus- EDNMR in these two donors. siontothesubharmonictransitionwhichshouldbemore To verify that residual RF magnetic fields (due to the robust against sample-specific strains. finite length of the device) can not be responsible for Spintransitionscannotbedrivensolelybymodulation the EDNMR, B(cid:126) was calibrated in the device using a of an isotropic hyperfine interaction due to the dispar- 2 Rabi-nutationexperimentandtheresultswerecompared ity in the electronic and nuclear precession frequencies. against the EDNMR data for both 31P and 75As. We AnytransitionmatrixelementsinvolvingA andA XX YY foundonewouldneed300timesmorepowerfortheresid- terms average out in the rotating wave approximation ual B(cid:126) fields to account for the EDNMR. andA termscannotdrivespinrotations. Wetherefore 2 ZZ To ensure that the subharmonic transitions were not require an anisotropic hyperfine interaction with A ZX artifactsdrivenbysecondharmonicsgeneratedintheRF terms to drive nuclear spins. To find the source of the source, the output of the RF source was fed directly into anisotropy, we turn to the spin-orbit Stark shift. aspectrumanalyzer. Weobservedthatintheworstcase We can compute the electric field modulation of gˆ us- configuration, a second harmonic was present and atten- ing the multivalley effective mass theory of [35] and the uated by 35 dB compared to the fundamental harmonic. experimentalStarkshiftvaluesfrom[20]and[36]asout- To further suppress this second harmonic, a set of sev- lined in the supplementary information. We find that enthorderButterworthlowpassfilters(CrystekCLPFL) the spin-orbit Stark shift directly modulates the quan- were used in every experiment, adding 35-50 dB of at- tization axis of the electron spin such that electron and tenuation. Given the more than 70 dB power difference nuclearspinsarequantizedalongdifferentaxes. RFelec- betweenthefirstandsecondharmonics,weareconfident tric fields then lead to RF modulation in the hyperfine that the observed subharmonic ENDOR transitions are field, as seen by the nuclear spin, which can lead to nu- not due to harmonics generated from the RF source. clear spin rotations. Totestthismechanismagainsttheexperiment,wede- veloped a model that simulates the Rabi-nutation ex- DISCUSSION periments in our device. This model accounts for ro- tation angle errors in both the ESR and NMR pulses, This is the first demonstration of electrically driven spin-resonator coupling, inhomogeneity in the RF and NMRfordonorsinsilicon. Wehaveidentifiedtwomecha- microwave fields, and the implant profile of the donors. nismsthatlikelyleadtotheobservedEDNMR,butmore Thissimulationtakesintoaccountvalleyrepopulationfor theoreticalandexperimentalworkwillbeneededtocon- electricfieldsinthe(100)crystallographicdirections(the firm our explanation. dominanteffect)butneglectsthe”singlevalley”effectde- To understand the EDNMR, we turn to the spin scribed in [35]. We find reasonable agreement with the Hamiltonian common to group V donors in silicon. This experimental data for the phosphorus donors as shown is given by inFig.4(c). Notethatthesimulationisplottedonadif- ferent voltage scale indicating a 4× discrepancy between H/h=βB(cid:126) ·gˆ ·S(cid:126)+S(cid:126)·Aˆ·I(cid:126)−β g B(cid:126) ·I(cid:126)+I(cid:126)·Qˆ·I(cid:126) (1) the simulation and data, which is reasonable given our 0 e n n 0 necessarily rough estimates of the parameters. However, where β is the Bohr magneton, gˆ is the electron gy- the equivalent 75As simulation (shown in supplementary e romagnetic tensor, S(cid:126) is the electronic spin, Aˆ is the hy- information) would require a 40× larger voltage which 5 implies that another mechanism must dominate. Our technique for controlling nuclear spins has several The only significantly different term in the 75As and advantages over magnetic control. It relaxes power re- 31P Hamiltonians is the quadrupolar coupling, so this quirements since voltages rather than currents are used, is a possible source for the discrepancy in the EDNMR and allows for high density, individually addressable ar- Rabi frequencies. It is difficult to determine transition rays of donor nuclear spins since electric fields are more frequencies for quadrupolar modulation, due to uncer- easilyconfinedthanmagneticfields. Sinceweareableto tainties in screening potentials from inner shell electrons drive spins at subharmonics of their resonance frequen- and no studies have reported electric field induced mod- cies and at subharmonics of double quantum ∆m = 2 I ulationofthequadrupolarinteraction. Therehave,how- transitions,ourelectricfieldcontrolmethodsubstantially ever, been several recent reports of quadrupolar shifts reduces the bandwidth requirements for quantum de- for 75As[38, 39] and 209Bi [40] donors in silicon subject vices while simultaneously expanding the computational to strain. By comparing the strain-induced hyperfine Hilbert space. From these results, one can envision new splitting measured in [39] to the hyperfine Stark data quantum computing architectures based on donor nu- of [36], we can approximately scale the experimentally clear spins in silicon. These techniques should extend to measured quadrupolar shifts in [39] to correspond to the other material systems with long coherence times such electric fields we apply in our experiments. By repeating as donors in germanium[42] which offer a four-order- the Rabi-nutation experiment simulations while includ- of-magnitude enhancement in the spin-orbit Stark shift ing the modulation of the quadrupolar interaction, the [21, 43]. The larger Stark effect should translate into Rabi frequencies are enhanced by more than a factor of significantly faster EDNMR gates. 10 as shown in Fig. 4(d). We find reasonable agreement We thank G. Pica, J. J. L. Morton, and P. Bertet to our data, again given the uncertainties in the param- for stimulating discussions. Work at Princeton was eters. We therefore conclude that the quadrupolar inter- supported by the NSF through the Princeton MRSEC action is most likely responsible for the spin transitions (Grant No. DMR-01420541) and by the ARO (Grant in 75As, however more theoretical work is warranted. No. W911NF-13-1-0179). WorkatLBNLwasperformed For the largest RF electric fields applied in this work, undertheauspicesoftheU.S.DepartmentofEnergyun- the average Rabi frequency is approximately 70 kHz for der Contract No. DE-AC02-205CH11231. the fundamental transition and 60 kHz for its subhar- monic. These applied fields are a factor of 10 below the donor ionization threshold [41], indicating that MHz fre- quencyEDNMRmanipulationsshouldbepossibleinun- strained Si. The fundamental transition Rabi frequen- ∗ [email protected] [1] R. P. 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The single (SQT) and double (DQT) quan- tumtransitionsarelabeledusingthegreennumbersandpink numerals, respectively. These labels are also used in (b-d). The Davies ENDOR spectra measured using magnetic (b) and electrical (c-d) RF pulses are plotted. The magnetically drivenENDORspectrashowsthesixSQTswhereastheelec- trically driven spectra (c) reveals both the SQTs and DQTs. Electrically driven ENDOR also resolves transitions at sub- harmonicsoftheSQTsasshownin(d). TheSQTsin(b)are power broadened. 8 FIG. 4. Rabi oscillations are recorded as a function of RF voltageamplitudefor31P(a)and75As(b)subharmonictran- sitions. The75Astransitionisat46.5MHzandthe31Ptran- sition is at 54 MHz. The simulated plots (c-d) show similar dependences to the data, but larger RF amplitudes must be assumed indicating that our models underestimate the tran- sition frequencies by a factor of 3-4. The phosphorus simu- lation takes into account g-tensor modulation leading to an anisotropichyperfinecouplingwhereasthearsenicsimulation also takes into account quadrupolar modulation. All data were taken at 1.9 K in a magnetic field of 250 mT.

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