quantum grade silicon - nist

11
Use of quantum effects as potential qualifying metrics for “quantum grade 1 silicon” 2 A. N. Ramanayaka, 1, 2 Ke Tang, 1, 2 J. A. Hagmann, 1 Hyun-Soo Kim, 1, 2 D. S. Simons, 1 C. A. Richter, 1 and J. M. 3 Pomeroy 1, a) 4 1) National Institute of Standards & Technology, Gaithersburg, Maryland 20899, 5 USA 6 2) Joint Quantum Institute, University of Maryland, College Park, Maryland 20742, 7 USA 8 (Dated: 10 December 2019) 9 Across solid state quantum information, materials deficiencies limit performance through enhanced relaxation, 10 charge defect motion or isotopic spin noise. While classical measurements of device performance provide cur- 11 sory guidance, specific qualifying metrics and measurements applicable to quantum devices are needed. For 12 quantum applications, new materials metrics, e.g., enrichment, are needed, while existing, classical metrics 13 like mobility might be relaxed compared to conventional electronics. In this work, we examine locally grown 14 silicon superior in enrichment, but inferior in chemical purity compared to commercial-silicon, as part of 15 an effort to underpin the materials standards needed for quantum grade silicon and establish a standard 16 approach for intercomparison of these materials. We use a custom, mass-selected ion beam deposition tech- 17 nique, which has produced isotopic enrichment levels up to 99.99998 % 28 Si, to isotopically enrich 28 Si, but 18 with chemical purity > 99.97% due the MBE techniques used. From this epitaxial silicon, we fabricate 19 top-gated Hall bar devices simultaneously on the 28 Si and on the adjacent natural abundance Si substrate 20 for intercomparison. Using standard-methods, we measure maximum mobilities of (1740 ± 2) cm 2 /(V · s) 21 at an electron density of (2.7 × 10 12 ± 3 × 10 8 ) cm -2 and (6040 ± 3) cm 2 /(V · s) at an electron density of 22 (1.2 × 10 12 ± 5 × 10 8 ) cm -2 at T =1.9 K for devices fabricated on 28 Si and nat Si, respectively. For magnetic 23 fields B> 2 T, both devices demonstrate well developed Shubnikov-de Haas (SdH) oscillations in the longitu- 24 dinal magnetoresistance. This provides transport characteristics of isotopically enriched 28 Si, and will serve 25 as a benchmark for classical transport of 28 Si at its current state, and low temperature, epitaxially grown Si 26 for quantum devices more generally. 27 Conventional electronics have been industrialized for 28 decades; consequently, precise metrics based on macro- 29 scopic properties, such as chemical purity, charge car- 30 rier mobility, defect density, are established for qualify- 31 ing a material, e.g., silicon, for conventional electronics. 32 While silicon has been the work horse of conventional 33 electronics, it also is becoming a promising host for spin 34 based quantum information processing devices. 1,2 Specif- 35 ically, spin qubits have already shown promising advance- 36 ments with regard to long coherence times, 3,4 manipula- 37 tion with high gate fidelity, 3,4 and scalability. 5,6 38 Even though silicon has improved tremendously over 39 the decades to meet demands of today’s state-of-the- 40 art transistors, this excellent material is still not suf- 41 ficient to support quantum information. For example, 42 in spin-based quantum information systems, the pres- 43 ence of the 29 Si isotope in natural abundance silicon re- 44 duces coherence times dues to the non-zero nuclear spin 45 of I =1/2. Nuclei with non-zero spin in the host lattice 46 act as a source of decoherence for spin based qubits, 7 47 as they interact with the electron spin through hyper- 48 fine interactions. 8,9 However, by placing a spin qubit in 49 an isotopically enriched 99.995 % 28 Si environment, 10 de- 50 velopment of silicon based quantum devices have gained 51 a) Correspondence to [email protected] considerable momentum, with reports of exceptionally 52 long quantum coherence times. 11,12 53 The need for some level of enrichment provides an ex- 54 ample of how “semiconductor grade” silicon quality may 55 be necessary, but is not sufficient to meet the needs of 56 quantum. Further, the metrics for conventional silicon 57 may not always be relevant for quantum, e.g., the ease 58 of carrier motion as quantified by mobility may not be 59 directly relevant to quantum device performance where 60 confinement and coherence in the absence of motion are 61 critical. Additionally, as we establish properties and their 62 numerical thresholds that are sufficient for quantum, rel- 63 atively simple qualifying metrics that act as general prox- 64 ies for properties more challenging to measure are invalu- 65 able. So, it may be that mobility in and of itself is not 66 important, but it could be a good proxy for estimating 67 spin-qubit relaxation or coherence. 68 As part of a larger program to identify and quantify 69 “quantum grade” silicon, we are identifying 1) proper- 70 ties beyond those considered for semiconductor grade sil- 71 icon critical to quantum; 2) the relevance and priority of 72 properties currently considered critical for semiconduc- 73 tors; and 3) standard methods that may be used for new 74 properties, or provide a general indicator for challenging 75 properties, e.g., coherence time; as three main goals that 76 are paramount for development of metrics for “quantum 77 grade” silicon. This work is part of a broader effort to 78 find ways besides making and measuring qubits to pro- 79 This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset. PLEASE CITE THIS ARTICLE AS DOI: 10.1063/1.5128098

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Page 1: quantum grade silicon - NIST

Use of quantum effects as potential qualifying metrics for “quantum grade1

silicon”2

A. N. Ramanayaka,1, 2 Ke Tang,1, 2 J. A. Hagmann,1 Hyun-Soo Kim,1, 2 D. S. Simons,1 C. A. Richter,1 and J. M.3

Pomeroy1, a)4

1)National Institute of Standards & Technology, Gaithersburg, Maryland 20899,5

USA6

2)Joint Quantum Institute, University of Maryland, College Park, Maryland 20742,7

USA8

(Dated: 10 December 2019)9

Across solid state quantum information, materials deficiencies limit performance through enhanced relaxation,10

charge defect motion or isotopic spin noise. While classical measurements of device performance provide cur-11

sory guidance, specific qualifying metrics and measurements applicable to quantum devices are needed. For12

quantum applications, new materials metrics, e.g., enrichment, are needed, while existing, classical metrics13

like mobility might be relaxed compared to conventional electronics. In this work, we examine locally grown14

silicon superior in enrichment, but inferior in chemical purity compared to commercial-silicon, as part of15

an effort to underpin the materials standards needed for quantum grade silicon and establish a standard16

approach for intercomparison of these materials. We use a custom, mass-selected ion beam deposition tech-17

nique, which has produced isotopic enrichment levels up to 99.99998 % 28Si, to isotopically enrich 28Si, but18

with chemical purity > 99.97% due the MBE techniques used. From this epitaxial silicon, we fabricate19

top-gated Hall bar devices simultaneously on the 28Si and on the adjacent natural abundance Si substrate20

for intercomparison. Using standard-methods, we measure maximum mobilities of ≈ (1740± 2) cm2/(V · s)21

at an electron density of (2.7× 1012 ± 3× 108) cm−2 and ≈ (6040± 3) cm2/(V · s) at an electron density of22

(1.2× 1012 ± 5× 108) cm−2 at T = 1.9 K for devices fabricated on 28Si and natSi, respectively. For magnetic23

fields B > 2 T, both devices demonstrate well developed Shubnikov-de Haas (SdH) oscillations in the longitu-24

dinal magnetoresistance. This provides transport characteristics of isotopically enriched 28Si, and will serve25

as a benchmark for classical transport of 28Si at its current state, and low temperature, epitaxially grown Si26

for quantum devices more generally.27

Conventional electronics have been industrialized for28

decades; consequently, precise metrics based on macro-29

scopic properties, such as chemical purity, charge car-30

rier mobility, defect density, are established for qualify-31

ing a material, e.g., silicon, for conventional electronics.32

While silicon has been the work horse of conventional33

electronics, it also is becoming a promising host for spin34

based quantum information processing devices.1,2 Specif-35

ically, spin qubits have already shown promising advance-36

ments with regard to long coherence times,3,4 manipula-37

tion with high gate fidelity,3,4 and scalability.5,638

Even though silicon has improved tremendously over39

the decades to meet demands of today’s state-of-the-40

art transistors, this excellent material is still not suf-41

ficient to support quantum information. For example,42

in spin-based quantum information systems, the pres-43

ence of the 29Si isotope in natural abundance silicon re-44

duces coherence times dues to the non-zero nuclear spin45

of I = 1/2. Nuclei with non-zero spin in the host lattice46

act as a source of decoherence for spin based qubits,747

as they interact with the electron spin through hyper-48

fine interactions.8,9 However, by placing a spin qubit in49

an isotopically enriched 99.995 % 28Si environment,10 de-50

velopment of silicon based quantum devices have gained51

a)Correspondence to [email protected]

considerable momentum, with reports of exceptionally52

long quantum coherence times.11,1253

The need for some level of enrichment provides an ex-54

ample of how “semiconductor grade” silicon quality may55

be necessary, but is not sufficient to meet the needs of56

quantum. Further, the metrics for conventional silicon57

may not always be relevant for quantum, e.g., the ease58

of carrier motion as quantified by mobility may not be59

directly relevant to quantum device performance where60

confinement and coherence in the absence of motion are61

critical. Additionally, as we establish properties and their62

numerical thresholds that are sufficient for quantum, rel-63

atively simple qualifying metrics that act as general prox-64

ies for properties more challenging to measure are invalu-65

able. So, it may be that mobility in and of itself is not66

important, but it could be a good proxy for estimating67

spin-qubit relaxation or coherence.68

As part of a larger program to identify and quantify69

“quantum grade” silicon, we are identifying 1) proper-70

ties beyond those considered for semiconductor grade sil-71

icon critical to quantum; 2) the relevance and priority of72

properties currently considered critical for semiconduc-73

tors; and 3) standard methods that may be used for new74

properties, or provide a general indicator for challenging75

properties, e.g., coherence time; as three main goals that76

are paramount for development of metrics for “quantum77

grade” silicon. This work is part of a broader effort to78

find ways besides making and measuring qubits to pro-79

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Page 2: quantum grade silicon - NIST

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vide diagnostics that will indicate the likely performance80

of qubits early in a fabrication stream.81

This paper presents devices, methods and results for82

a comparative study of magnetotransport properties be-83

tween 1) high isotopic enrichment, low chemical purity84

and 2) high chemical purity, natural abundance (low iso-85

topic enrichement) silicon. This characterization sets the86

stage for determining whether coherence properties in87

quantum dot devices correlate with the trends in these88

simpler measurements, since the benefit of enrichment on89

coherence may outpace the liability of some additional90

contaminants. In a detailed theoretical study, Witzel et91

al.,13 illustrate that the coherence of a spin qubit can,92

in principle, be increased by an order of magnitude for93

every order of magnitude increase in the isotopic enrich-94

ment of 28Si in the qubit’s Si environment. A comprehen-95

sive experimental investigation of this prediction, how-96

ever, is hindered due to the discreteness of the available97

isotopic enrichment levels. Among the four different en-98

richment levels have been reported10,14–16 only 99.98%99

28Si14 and 99.995% 28Si10 have been utilized for quantum100

electronic device fabrication.11,17,18 Moreover, contem-101

porary methods for producing isotopically enriched 28Si102

material are based on chemical vapor deposition (CVD)103

techniques and are not compatible with qubit architec-104

tures requiring low temperature processing, e.g. STM105

fabricated single dopant atom qubits.19 In contrast, the106

method used for producing 28Si reported here is compat-107

ible with all the contemporary qubit architectures, and108

represents molecular beam epitaxy (MBE) grown Si more109

generally. While the coherence of a spin qubit is pre-110

dicted to improve at higher isotopic enrichment levels,13111

how other material properties will limit the expected en-112

hancement of qubit coherence is unclear. To the best of113

our knowledge, no study yet has attempted to correlate114

macroscopic electrical characteristics to the performance115

of quantum devices. Yet such a study will be an essen-116

tial component for defining metrics for “quantum grade”117

silicon within the three main goals identified earlier.118

Starting from natural abundance SiH4 gas, we have119

developed a method to grow isotopically purified silicon120

reaching isotopic enrichments up to 99.99998 % 28Si.20,21121

This method provides the unique advantage of targeting122

a desired enrichment level anywhere from natural abun-123

dance to the highest possible enrichment.22 As a first124

step towards correlating macroscopic electrical charac-125

teristics with the performance of quantum devices, we126

report here on characterization of gated Hall bar de-127

vices fabricated on isotopically enriched 28Si, and con-128

trol devices on the same natural abundance Si (natSi)129

substrate but outside the isotopically enriched 28Si spot130

using macroscopic manifestations of quantum effects such131

as Shubnikov-de Haas (SdH) effect and weak-localization132

effect. We compare the devices fabricated on natSi (float-133

zone grown) and 28Si (MBE grown) during the same fab-134

rication process, eliminating possible differences due to135

imperfect fabrication conditions. We present results of136

28Si devices to serve as a benchmark for MBE grown iso-137

0 50 100 150 200

10-4

10-3

10-2

10-1

Isoto

pic

ratio 2

9S

i/2

8S

i

Natural Si

1

2

3

Depth (nm)

(a)

natSi substrate

Enriched 28Si

Gate oxide(60 nm SiO2)

P implant

Ohmic contact

Top gate

200 μm

(c)

Top gate

P implants

Ohmic contacts

(d)

12

3

(b)

natSi

Deposited 28Si spot

Si handle (4 × 10) mm Devices

FIG. 1. (a) A schematic illustrating the device layout of agiven sample. Reduced coverage of the 28Si spot allows to fab-ricate devices on 28Si and natSi simultaneously. (b) Schematicrepresentation of the gated Hall bar device fabricated on 28Siis shown. (c) An optical micrograph of a gated multi-terminalHall bar device fabricated on 28Si is shown.(d) The isotopicratios of 29Si/28Si at positions 1 (4), 2 (©), and 3 (�) in (c)are shown. The shift in the rising edge at different positionscorresponds to the thickness variation in the deposited 28Sifilm. Measured 29Si isotopic ratios at locations 1, 2, and 3 are(149± 18)× 10−6 mol/mol, (128± 14)× 10−6 mol/mol, and(45± 2)× 10−6 mol/mol, respectively.

topically enriched 28Si, and a basis for comparing macro-138

scopic electrical characteristics within silicon quantum139

electronics.140

Starting with 99.999 % pure, commercially available,141

natural isotopic abundance SiH4 gas, isotopically en-142

riched 28Si is grown using a hyperthermal energy ion143

beam deposition system20. Gated Hall bar devices are144

fabricated on isotopically enriched 28Si epilayers in or-145

der to electrically characterize the material. Typically,146

the isotopically purified 28Si spot is ≈ 2 mm2 to 3 mm2147

in area and covers only a small fraction of the starting148

float-zone grown, natural abundance, intrinsic Si sub-149

strate (4 mm× 10 mm), see Fig. 1(a). Due to the re-150

duced coverage of the 28Si spot, devices on isotopically151

enriched and natural abundance Si can be fabricated on152

the same Si chip [see Fig. 1(a)] at the same time. This153

eliminates the effect of imperfections in the fabrication154

process (e.g., oxide growth) when comparing the electri-155

cal properties of the devices. A schematic cross section156

of a device fabricated on 28Si spot is shown in Fig. 1(b).157

The structure of the devices fabricated on natSi, i.e. out-158

side the 28Si spot, is identical except without the 28Si159

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TABLE I. Macroscopic materials and electrical properties ofnatural abundance, natSi, and isotopically enriched, 28Si, sil-icon.

PropertyMaterial

natSi 28Si

Avg. 28Siconcentration 92.23 % 99.983 %

Impurities (cm−3)C

≤ 10162× 1019

N 3× 1017

O 3× 1018

Max. mobilityµ (cm2/(V · s)) (6040± 3) (1740± 2)Percolation densitynp (1011 cm−2) (2.3± 2) (4.2± 2)

layer. An optical micrograph of the gated multi-terminal160

Hall bar device is shown in Fig. 1(c).161

The isotopic enrichment of the 28Si epilayers is162

measured by using Secondary Ion Mass Spectrometry163

(SIMS). In Fig. 1(d), the SIMS-derived isotopic ratio164

of 29Si/28Si is shown as a function of depth at several165

locations near the fabricated Hall bar device. For the de-166

vice reported here, the level of isotopic enrichment mea-167

sured at locations 1, 2, and 3 corresponds to ≈ 99.976 %,168

≈ 99.980 %, and ≈ 99.993 % 28Si, respectively. Figure169

1(d) also reveals the thickness non-uniformity of the170

deposited 28Si epilayer, i.e., the thickness of the 28Si171

epilayer at location 3 is greater than that of locations172

1 and 2. Moreover, separate SIMS measurements on173

these isotopically enriched 28Si epilayers reveals that the174

films contain adventitious chemical impurities, namely175

C, N, O, with approximate atomic concentrations of176

2× 1019 cm−3, 3× 1017 cm−3, and 3× 1018 cm−3. How-177

ever, the atomic concentrations of these chemical impu-178

rities on the handle wafer were below the SIMS detection179

limit (≤ 1016 cm−3). We believe that these chemical im-180

purities are being introduced by the ion beam as result181

of non-UHV compatible ionization source that is used182

to create the ion beams during the 28Si deposition, and183

since been upgraded.184

The magnetoresistance (Rxx) and the Hall resistance185

(Rxy) at 1.9 K for isotopically enriched 28Si and natural186

abundance Si are shown in Fig. 2(a) and Fig. 2(b), re-187

spectively. Using low field magnetotransport data, we188

find maximum mobilities at T = 1.9 K for 28Si and189

natSi are, respectively, µ28Si = (1740± 2) cm2/(V · s)190

at an electron density n of (2.7× 1012 ± 3× 108) cm−2191

and µnatSi = (6040± 3) cm2/(V · s) at an electron den-192

sity of (1.2× 1012 ± 5× 108) cm−2. Charge carrier mo-193

bilities for these devices are within the typical range194

of mobilities for Si-MOS (Metal Oxide Semiconduc-195

tor) devices fabricated using non-MBE (e.g. CVD)196

growth techniques,23,24 the maximum mobility for a Si-197

MOS device to date being > 4× 104 cm2/(V · s)25. In198

contrast, mobilities reported for Si-MOS devices fabri-199

-10 -5 0 5 10-6000

-4000

-2000

0

2000

4000

6000

0

200

400

600

800

1000

1200

Rxx (

)

On chip natural abundance Si

Rxy (

)

B (T)

T=1.9 K, Vg=8 V

=

-10 -5 0 5 10-3000

-2000

-1000

0

1000

2000

3000

1100

1200

1300

1400

T=1.9 K, Vg=8 V

Isotopically enriched 28Si

Rxx (

)

=

Rxy (

)

B (T)

(a)

(b)

FIG. 2. The magnetoresistance Rxx (right-axis) and the Hallresistance Rxy (left-axis) measured for the devices fabricatedon (a) isotopically enriched 28Si epi-layer, and (b) naturalSi substrate are shown. For both devices, the correspondingfilling factors (ν) are shown at the minima of Shubnikov-deHass oscillations. In contrast to the device on isotopicallyenriched 28Si epi-layer, the device on natSi demonstrates spin-splitting for B > 3 T. Both devices are fabricated on thesame Si chip, see main text for more information. The relativeuncertainty associated with Rxx and Rxy is typically less than0.1 % and is mostly due to the uncertainty of the measuredcurrent.

cated on MBE grown Si ranges from 900 cm2/(V · s) to200

1250 cm2/(V · s)26,27.201

In order to estimate the percolation electron density202

np, we extrapolate the electron density as a function of203

gate voltage (as determined from Hall measurements)204

back to the threshold voltage (as determined from the205

channel current Isd vs. Vg), i.e., np = ne(Vth). Using206

this method, we find percolation densities of (2.3± 2)×207

1011 cm−2 for natSi and (4.2 ± 2) × 1011 cm−2 for 28Si.208

While the relative uncertainties are large due to the ex-209

trapolation, we think the ≈ 2× larger value for 28Si is210

significant. A summary of these macroscopic materials211

and electrical properties for the on-chip natSi and 28Si is212

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Page 4: quantum grade silicon - NIST

4

provided in table I.213

Both devices show well developed SdH oscillations in214

Rxx with accompanying plateaus in Rxy. The slight215

asymmetry in Rxx in Fig. 2(a) could be due to sev-216

eral reasons, e.g., magnetic impurities or inhomogeneity217

of the magnetic field.28,29 The SIMS of a similar 28Si epi-218

layer found no measurable magnetic impurities. The Hall219

resistance shows non-idealities particularly in the natSi220

device [Fig. 2(b)] where Rxy is non-monotonic. These221

non-idealities could be due to scattering between discrete222

degenerate states at the tails due to level broadening.30,31223

However, a detailed discussion of the asymmetry of Rxx224

and the flatness of the Hall plateaus is outside the scope225

of this article. We also see a lifting of the four-fold de-226

generacy at B > 5 T for natSi, which is likely due to the227

spin degree of freedom, but, at this time we are unable228

to determine whether this is due to spin or valley degree229

of freedom, due to limitations in the experimental setup.230

Near zero magnetic field, both devices demonstrate231

a peak in the sample resistance, see Fig. 2. This in-232

crease in resistance near zero magnetic field is known as233

weak localization (WL). Weak localization is a quantum234

mechanical phenomenon that can be observed in two-235

dimensional (2D) electron systems at low temperatures236

where the phase coherence length (lφ) is greater than237

the mean free path (l)32,33. Relative to the zero field238

resistance, the weak-localization is larger for the device239

fabricated on isotopically enriched 28Si.240

To further investigate the WL behavior of these de-241

vices, we plot the change in conductivity ∆σxx as a func-242

tion of magnetic field B applied perpendicular to the 2D243

electron system [see Fig. 3]. The change in conduc-244

tivity due to WL ∆σxx = σxx(B)− σxx(B = 0), where245

σxx = ρxx/(ρ2xx + ρ2

xy). For non-zero B, the change246

in conductivity due to WL in a 2D electron system247

can be modeled by the Hikami-Larkin-Nagaoka (HLN)248

equation,34249

∆σxx(B) =α( e2

2π2~

)[Ψ(1

2+

~4el2φB

)−Ψ(1

2+

~2el2B

)− ln

( l

2lφ

)], (1)

where Ψ is the digamma function, l is the mean free250

path, lΦ is the phase coherence length, and α is a con-251

stant close to unity. In Fig. 3, the solid lines are the252

fits to experimental data (symbols) using the HLN equa-253

tion. For these fits, we use the calculated values of l254

TABLE II. Parameters extracted from the least-squares-fitsof Eq. 2 to the data in Fig. 3 inset.

Devicea b c Adjusted

(1010 s−1) (1010 K−1s−1) (1010 K−2s−1) R-square

28Si 6.6± 2 3.1± 0.7 0.60± 0.08 0.997natSi 5.1± 0.4 - 1.5± 0.1 0.989

0.0 0.1 0.2 0.30

2

4

6

8

10

12

14

16

18

28Si

natSi

HLN fits

xx (

S)

B (T)

T = 3 K 2 4 6 8 10

2

4

6

8

10

12 28Si

natSi

fit

1/ (

10

11/s

)

T (K)

FIG. 3. The change in conductivity (∆σxx) vs external mag-netic field (B) for devices fabricated on 28Si (�) and natSi(©) measured at 3 K. Solid lines are the least-square-fits toHLN equation (Eq. 1). Estimated uncertainty for ∆σxx is< 0.3 %. Inset: The inelastic scattering rates (1/τφ) for 28Siand natSi vs the measurement temperature are shown. Herethe solid lines are the least-squares-fit to a quadratic equa-tion, see main text details. Error bars in the inset representthe fit uncertainty associated with the values extracted for1/τφ at each temperature.

using the relation l =√

2Dτ . Here D is the diffusion co-255

efficient defined as D = v2F τ/2, where the Fermi velocity256

vF = ~kF /m∗, and τ is the elastic scattering time, also257

known as transport lifetime, defined as τ = µm∗/e. The258

effective mass m∗ is defined as m∗/m0 = 0.19, where m0259

is the rest mass of an electron.35,36 The Fermi wavelength260

kF can be calculated for a 2D electron system in Si as261

kF = (4πn2D/gsgv)1/2, where n2D, gs, gv are the charge262

carrier density, spin degeneracy and valley degeneracy,263

respectively. We leave α and lφ as free fitting param-264

eters, constraining the value of α to be close to unity.265

From the fit-extracted values of lφ, we calculate 1/τφ,266

where inelastic scattering time τφ = l2φ/D. The fit de-267

rived values of 1/τφ as a function of T are plotted in268

Fig.3 inset for devices fabricated on isotopically enriched269

28Si and natural abundance Si, respectively. The solid270

lines in Fig. 3 inset are the least-squares-fit to the data271

using the equation272

1

τφ= a+ bT + cT 2. (2)

The linear in T term captures the scattering from im-273

purities, and the quadratic in T term is related to the274

electron-electron scattering.37 Table II shows the param-275

eters extracted from the least-squares-fit to the data, the276

fit uncertainties for both devices, and the adjusted R-277

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(a)

(b) (c)

2 4 60.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

(p

s)

q (28Si)

(28Si)

q (natSi)

(natSi)

T (K)

0.1 0.2 0.30

1

2

3

4

5 28Si

fit

ln(A

SdH/X

(T))

1/B (1/T)

T = 3 K

0.1 0.2 0.3

1200

1250

1300

T = 3 K

Rxx (

)

1/B (1/T)

Amplitude (ASdH)

Isotopically enriched 28Si

FIG. 4. (a) The background subtracted (see text) Rxx,i.e., ∆Rxx, vs the inverse of the external magnetic field(1/B) for the 28Si device is shown. (b) A “Dingle plot” ofln(ASdH/X(T )) versus 1/B. Error bars represent the uncer-tainty associated with extracting ASdH from ∆Rxx vs. 1/Bplot. (c) The single particle lifetimes, τq, extracted from theDingle plots and transport lifetimes, τ , at different temper-atures for devices on 28Si and natSi. Error bars representthe uncertainty associated with calculating the values of τq(τ) using the Dingle plots (charge carrier mobilities) at eachtemperature.

square. For the natural abundance Si, the best fit is278

achieved when the linear term is set to zero, i.e., b = 0.279

Consequently, for natural abundance Si the dominant280

scattering mechanism appears to be the electron-electron281

(long-range) scattering. In contrast, for isotopically en-282

riched 28Si, the best fit is achieved with a significant283

linear in T term. This large linear term implies that284

impurity (short-range) scattering is a significant contri-285

bution in 28Si. The temperature independent parameter286

a is similar (within the uncertainties) for both the de-287

vices indicating the processes (e.g., interface roughness)288

contributing to a are likely the same.289

Line shape analysis of the SdH oscillations as a290

function of temperature is also used to investigate291

the underlying scattering mechanisms in 2D electron292

systems. The amplitude of the SdH oscillations can293

be written as ASdH = X(T )R0exp(−π/ωcτq)38,39,294

where R0 is the zero field resistance,295

X(T ) = (2π2kBT/~ωc)/ sinh(2π2kBT/~ωc) is the296

temperature damping factor, and ωc = eB/m∗ is the297

cyclotron frequency. Here, kB is Boltzmann’s constant,298

and τq is the single particle (quantum) lifetime.38–40299

To extract the amplitude of SdH oscillations, we first300

subtract a slow varying background from Rxx41 to isolate301

the oscillatory part of Rxx. The Rxx after background302

subtraction (∆Rxx) is plotted against 1/B in Fig. 4(a).303

Then we extract the amplitude ASdH as schematically304

defined in Fig. 4(a) at each minima of ∆Rxx and305

calculate ln(ASdH/X(T )). Figure 4(b) is a plot of306

ln(ASdH/X(T )) versus 1/B, also known as the “Dingle307

plot”38,39 for the device fabricated on 28Si measured308

at T = 3 K. The approximately linear dependence of309

ln(ASdH/X(T )) on 1/B [see Fig. 4 (b)] indicates a310

magnetic field independent quantum lifetime, τq. In311

Fig. 4 (c), we plot the quantum lifetimes, τq, for devices312

fabricated on 28Si and natSi extracted from a linear313

least-squares-fit to Dingle plots at each temperature.314

The calculated values of the transport lifetimes, where315

τ = µm∗/e, using the magnetotransport measurement316

at low magnetic fields for both devices, are also plotted317

in Fig. 4 (c).318

For the device fabricated on 28Si, the ratio of τ/τq ≈ 1,319

and for the device on natSi the ratio of τ/τq ≈ 1.4. The320

transport lifetime τ is primarily affected by the large an-321

gle scattering events that cause large momentum change,322

whereas τq is affected by all of the scattering events42.323

When the background impurities dominate the scattering324

the ratio τ/τq is less than or equal to 10, whereas it is ≈ 1325

when the scattering is dominated by short-range isotropic326

scattering42, e.g. surface roughness scattering43. The327

thickness of the gate oxide for the devices reported here328

is ≈ 60 nm. We therefore neglect the scattering due to re-329

mote interface roughness (i.e., the interface between the330

gate oxide and the gate metal) as a dominant scatter-331

ing mechanism for these devices.44 Therefore, the ratio332

τ/τq implies that the charge carrier mobility is limited by333

the background impurity scattering. Furthermore, the334

charge carrier mobility of the device on isotopically en-335

riched 28Si may also be limited by the interface roughness336

scattering.337

The analysis of the weak-localization, SdH oscilla-338

tions, and low-field magnetotransport data indicate that339

the shortest scattering length scale to be the elastic340

(transport) scattering length l calculated, ≈ 33 nm and341

≈ 71 nm for 28Si and natSi, respectively. Capacitance342

voltage (CV) measurements of MOS capacitors fabri-343

cated on natural abundance silicon (data not shown) with344

gate oxides grown using similar conditions to the devices345

reported here reveals a fixed charge density of approxi-346

mately 3× 1010 cm−2 corresponding to a nearest neigh-347

bor distance of ≈ 58 nm. This nearest neighbor distance348

is in close agreement with the transport scattering length349

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6

l. Considering SIMS measured chemical impurity con-350

centrations of C, N, and O and assuming these impurities351

acting as isolated scatters, for 28Si where l ≈ 33 nm, we352

estimate the fraction of C, N, and O impurities contribut-353

ing to scattering to be ≈ 0.2 %, ≈ 9.3 % and ≈ 1.0 %,354

respectively.355

In conclusion, we have reported on the first low tem-356

perature electrical measurements of MBE grown isotopi-357

cally enriched 28Si. For this report we fabricated and358

characterized the low temperature magnetotransport of359

gated Hall bar devices fabricated on highly enriched 28Si.360

In comparison to control devices fabricated on float-zone361

grown, intrinsic, natural abundance Si on the same sub-362

strate, the charge carrier mobility on isotopically en-363

riched 28Si is approximately a factor of 3 lower. Neverthe-364

less, the magnetotransport measurements of devices fab-365

ricated on isotopically enriched 28 Si demonstrate strong366

manifestations of quantum effects. Based on the analysis367

of temperature dependence of the weak localization and368

SdH oscillations, we believe that the dominant scatter-369

ing mechanism is short-range scattering (impurity scat-370

tering). We believe adventitious chemical impurities de-371

tected in the 28Si epilayers act as the impurity scatters in372

the devices fabricated on 28Si. However, higher levels of373

adventitious chemical impurities detected in the 28Si epi-374

layers are too high to be considered as isolated scattering375

centers, since the nearest neighbor distance is consider-376

ably shorter than the scattering lengths extracted from377

the transport data. Further, for these impurity levels,378

the dipolar interactions between randomly distributed379

electron spins associated with impurities and the central380

spin of a potential qubit is considered to be the domi-381

nant decoherence mechanism at high enrichments.13 For382

the worst case analysis, if all of the N and O chemical383

impurities are considered as randomly distributed single384

electron spins, the influence of these dipolar interactions385

on the central spin could result in qubit coherence times386

poorer than high purity natural abundance Si. However,387

we are confident that the recent and planned improve-388

ments, as well as techniques for depleting impurities near389

the surfaces, will allow us to move forward and study the390

tension between chemical impurites and enrichement on391

quantum coherence.392

Next we plan to fabricate quantum dot devices on con-393

trol (natural abundance) and isotopically enriched 28Si394

to more rigorously assess the impact of purity and en-395

richment, e.g. charge offset drift, as the chemical purity396

of these MBE grown 28Si films is improved. Therefore,397

macroscopic transport and material characteristics of the398

devices reported here will serve as a benchmark for find-399

ing the correlations between macroscopic properties and400

the performance of future nanoscale devices, e.g. quan-401

tum dots, and lead to identifying qualifying metrics for402

“quantum grade” silicon.403

ACKNOWLEDGMENTS404

The authors acknowledge stimulating discussions with405

Michael Stewart, Neil Zimmerman, Roy Murray, Ryan406

Stein, Binhui Hu, and Peihao Huang.407

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0 50 100 150 200

10-4

10-3

10-2

10-1

Isoto

pic

ratio 2

9S

i/2

8S

i

Natural Si

1

2

3

Depth (nm)

(a)

natSi substrate

Enriched 28Si

Gate oxide(60 nm SiO2)

P implant

Ohmic contact

Top gate

200 μm

(c)

Top gate

P implants

Ohmic contacts

(d)

12

3

(b)

natSi

Deposited 28Si spot

Si handle (4 × 10) mm Devices

Page 9: quantum grade silicon - NIST

-10 -5 0 5 10-6000

-4000

-2000

0

2000

4000

6000

0

200

400

600

800

1000

1200

Rxx (

)

On chip natural abundance Si

Rxy (

)

B (T)

T=1.9 K, Vg=8 V

=

-10 -5 0 5 10-3000

-2000

-1000

0

1000

2000

3000

1100

1200

1300

1400

T=1.9 K, Vg=8 V

Isotopically enriched 28Si

Rxx (

)

=

Rxy (

)

B (T)

(a)

(b)

Page 10: quantum grade silicon - NIST

0.0 0.1 0.2 0.30

2

4

6

8

10

12

14

16

18

28Si

natSi

HLN fits

xx (

S)

B (T)

T = 3 K 2 4 6 8 10

2

4

6

8

10

12 28Si

natSi

fit

1/ (

10

11/s

)

T (K)

Page 11: quantum grade silicon - NIST

(a)

(b) (c)

2 4 60.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

1.0

(p

s)

q (28Si)

(28Si)

q (natSi)

(natSi)

T (K)

0.1 0.2 0.30

1

2

3

4

5 28Si

fit

ln(A

SdH/X

(T))

1/B (1/T)

T = 3 K

0.1 0.2 0.3

1200

1250

1300

T = 3 K

Rxx (

)

1/B (1/T)

Amplitude (ASdH)

Isotopically enriched 28Si