Supplementary Information Gate-tunable quantum oscillations in ambipolar Cd3As2 thin films Yanwen Liu1,2, Cheng Zhang1,2, Xiang Yuan1,2, Tang Lei1, Chao Wang3, Domenico Di Sante4,5, Awadhesh Narayan6,7, Liang He8,9, Silvia Picozzi4, Stefano Sanvito6, Renchao Che3, Faxian Xiu1,2 1 State Key Laboratory of Surface Physics and Department of Physics, Fudan University, Shanghai 200433, China 2 Collaborative Innovation Center of Advanced Microstructures, Fudan University, Shanghai 200433, China 3 Department of Materials Science and Advanced Materials Laboratory, Fudan University, Shanghai 200433, China 4 Consiglio Nazionale delle Ricerche (CNR-SPIN), Via Vetoio, L'Aquila, Italy 5 Department of Physical and Chemical Sciences, University of L'Aquila, Via Vetoio 10, I-67010 L'Aquila, Italy 6 School of Physics, CRANN and AMBER, Trinity College, Dublin 2, Ireland 7 Department of Physics, University of Illinois at Urbana-Champaign, Illinois, USA 8 National Laboratory of Solid State Microstructures, School of Electronic Science and Engineering, Nanjing University, Nanjing 210093, China 9 Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China Correspondence and requests for materials should be addressed to F. X. and R. C. (E-mails: faxian@fudan.edu.cn and rcche@fudan.edu.cn) 1 I. Sample descriptions Several as-grown thin film samples have been measured with ionic gating. Sample Q1 is the sample described in the main text for positive gate voltages and SdH oscillations (Fig. 2c, the electron density in Fig. 3e, Fig. 4 and Fig. 5). Sample Q6 shows a systematic hole carrier transport in the main text (Fig. 2d, Fig. 3). The results of samples Q2~Q5 are summarized in the Supplementary Section VII (Fig. S12-17). All these samples exhibit the similar transport properties. II. Hopping conduction a b c 4.12 4.26 Q2 -1.25 V Q1 -1.5 V 4.10 Q6 -0.6 V 4.10 4.08 log(R) log(R) log(R) 4.24 4.08 4.06 4.06 4.20 4.04 4.04 4.22 4.02 0.3 0.4 0.5 0.6 0.7 0.8 T-1/3 (K-1/3) 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.3 T-1/3 (K-1/3) 0.4 0.5 0.6 0.7 T-1/3 (K-1/3) Figure S1| Hopping transport of Cd3As2 thin films at low temperatures under several gate voltages. III. Gating effect of Cd3AS2 thin films with solid electrolyte The gate sweeping process was carried out at 290 K, slightly higher than the frozen point of solid electrolyte (~280 K). The on-off ratio at 290 K is about 5 (Fig. S2), while at low temperatures it could increase to about 30 (Fig. S4). We believe that by reducing the dimensionality, the band gap can be slightly enlarged which results in the improved on-off ratio. The carrier density and mobility show negligible temperature dependence below 60 K (Fig. S3a-b). The behavior is similar to that of MoS2 devices encapsulated by 2 0.8 hBN1. It is probably attributed to the reduction of impurity scattering because the solid electrolyte serves as a top gate. Figure S2 | Rxx-Vg curve at 290 K of sample Q1 (black one). The sweep rate of gate voltage is 1 mV/s. The leakage current (blue curve) is negligible and therefore the electrostatic doping effect is dominated during the experiments. b 10 0.2 0.7 3500 0.3 0.9 8 6 4 3000 2500 Vg (V) 2000 2 10 100 T (K) nhall (×1012 cm-2) 10 0 0.5 1.2 μhall (cm2V-1s-1) nhall (×1012 cm-2) 12 c Vg (V) 0 0.2 0.5 0.9 0.3 0.7 1.2 10 nhall 3600 μhall 9 3400 8 7 3200 6 3000 5 4 2800 3 2600 2 100 0.0 T (K) 0.2 0.4 0.6 0.8 1.0 1.2 Vg (V) Figure S3 | Carrier density and mobility obtained from the Hall effect measurements (sample Q1). a, Temperature-dependent carrier density under different gate voltages. b, Temperature-dependent mobility under different gate voltages. Both the carrier density and mobility are nearly temperature independent below 60 K. c, Gate-dependent carrier density and mobility at 4 K. 3 2400 μhall (cm2V-1s-1) a b 14000 Q1 9000 10000 8000 20000 Q6 15000 R (Ω) R (Ω) 12000 c Q2 12000 R (Ω) a 6000 10000 5000 6000 3000 0 4000 0 -2.2 -2.0 -1.8 -1.6 -1.4 -1.2 -1.0 -2.5 -2.0 Vg (V) -1.5 -1.0 -0.5 Vg (V) 0.0 -2.5 -2.0 -1.5 -1.0 Vg (V) Figure S4| Resistance at 2 K of the Cd3As2 thin films. a, Id-Vg curve of sample Q1 (in the main text). b, Id-Vg curve of sample Q2. The detailed quantum oscillations are shown in the Supplementary Section V. When Vg<-2V, the saturation was observed. c, Id-Vg curve of sample Q6. The ambipolar behavior and the hole-dominated transport are clearer owing to the increased the area of the gate electrode and the reduced area of channel. IV. Two carrier transport of Cd3As2 thin films With negative gate voltages, hole carriers are electrostatically doped into the thin films, shifting the Fermi level towards the valence band. Both electrons and holes contribute to the transport. We note that at the turning points of the Hall slopes (Fig.S5a-d), the MR curves also show the change of curvature as marked by the arrows, giving another evidence of the two carrier transport in our Cd3As2 films. With the two-carrier transport equation, the carrier density and mobility of holes and electrons could be obtained. Fig. S5c and d show two fitting curves of the Hall data with red dash lines for sample Q1, and the fitting results are summarized in Fig. S7. Similar analyses have been applied to sample Q6 (Fig. S8). From the Kohler’s plot2–4 as explained in the main text, we could also identify the two carrier transport distinctly (see the Kohler’s plots in Fig. S6e-f for sample Q1 and Fig. S9 for sample Q6). It is interesting that the Kohler’s plot of MR at 0 V doesn’t fall on a universal curve at high field (Fig. S6d). However, with the linear Hall slopes at high field (not 4 -0.5 0.0 shown here), it does not show the two carrier transport but exhibits anisotropy of scattering time at the Fermi surface. The shadowed area marks the regime where the Kohler’s rule is obeyed at low field. The shadowed area increases as the gate voltage increasing (Fig. S6c-d), suggesting the reduction of the anisotropy. The results agree with the observed dipolar pattern in the polar plots in Fig.5c of the main text. The curves at 4 K deviate from the universal curve because of the quantum oscillations. With increasing carrier density, the influence from orbit quantization is enhanced, making the Kohler’s rule break down3,4 (Fig. S6a-b). In the Kohler’s plot of 1.2 V, the curves have similar trend but a little shift from each other, different from the disorder in the Kohler’s plot at negative gate voltage (Fig. S6e-f). The violation here doesn’t explicitly mean the anisotropy of Fermi surface. a b 8 4 Vg=-1 V Vg=-1.5V 30 10 Rxy Rxy 4 2 0 Rxy (kΩ) 0 Rxx (kΩ) 8 Rxy (Ω) Rxx (kΩ) 25 20 Rxx Rxx -4 -2 6 15 -8 -4 -2 0 2 4 6 8 -8 -8 B (T) -6 -4 -2 2 4 6 8 1.5 Vg=-1.8 V Vg=-2 V 14 1.0 1.0 22 0.5 20 13 0.0 18 Rxx (kΩ) Rxy Rxy (Ω) Rxx (Ω) -4 B (T) d 24 0 0.5 Rxx 0.0 Rxy 12 -0.5 -0.5 16 Rxy (kΩ) c -6 Rxx 11 -1.0 14 -1.0 -8 -6 -4 -2 0 2 4 6 10 8 B (T) -8 -6 -4 -2 0 B (T) 5 2 4 6 8 -1.5 Figure S5 | Two carrier transport of sample Q1. MR and Hall under 4 K at the gate voltage of -1 V (a), -1.5 V (b), -1.8 V (c) and -2V (d), respectively. The blue lines are the Hall data and the black lines are the MR data. The red dash lines in c and d are the fitting curves of two-carrier model. a c b 0.20 0.5 Vg= 1.2 V 4K 20K 30K 40K 60K 80K 0.05 0.00 0.0 1.0x10-4 2 xx 2 0.5 0.4 Vg=0 V 4K 20K 30K 40K 60K 80K 0.2 0.1 0.0 0 1x10-5 2 2x10-5 2 2 3x10-5 -2 B /Rxx(0) (T Ω ) 4x10-5 ΔRxx(B)/Rxx(0) ΔRxx(B)/Rxx(0) e 0.6 0.3 2.0x10-5 2 4.0x10-5 2 xx 6.0x10-5 2 -2 0.4 0.3 Vg =0.2 V 4K 20K 30K 40K 60K 80K 0.2 0.1 0.0 8.0x10-5 0 B /R (0) (T Ω ) B /R (0) (T Ω ) d 4K 20K 30K 40K 60K 80K 0.1 0.0 0.0 3.0x10-4 2.0x10-4 2 -2 Vg=0.5 V 0.2 f 0.8 0.6 0.4 Vg=-1.8 V 2K 10K 20K 40K 80K 120K 0.2 0.0 0.0 2 2 5.0x10-7 2 -2 B /Rxx(0) (T Ω ) 1x10-5 2x10-5 3x10-5 4x10-5 5x10-5 6x10-5 2 -2 2 2 xx B /R (0) (T Ω ) ΔRxx(B)/Rxx(0) 0.10 0.3 ΔRxx(B)/Rxx(0) 0.15 ΔRxx(B)/Rxx(0) ΔRxx(B)/Rxx(0) 0.4 0.6 0.4 Vg=-2 V 2K 10K 20K 40K 80K 120K 0.2 0.0 0.0 5.0x10-7 B2/Rxx(0)2 (T2Ω-2) Figure S6 | The Kohler’s plots of the MR curves of sample Q1 at the gate voltage of 1.2 V (a), 0.5 V (b), 0.2 V(c), 0 V (d), -1.8 V (e) and -2 V (f), respectively. If there is a single type of charge carrier with the same scattering time at the Fermi surface everywhere, the temperature-dependent Kohler plot of MR curve would overlap each other. Here the non-overlapping behavior in e and f along with the non-linear Hall data suggests unambiguously two-carrier transport. The non-overlapping behavior in e suggests different scattering time at the Fermi surface. 6 1.0x10-6 b Vg=-1 V 150K 80K 40K 20K 10K 2K 6000 4000 0 120K 80K 40K 20K 10K 2K 2000 Rxy (Ω) Rxy (Ω) 2000 Vg=-1.5 V 4000 e 10 8 6 4 0 2 -2 -2000 -1 -2000 -4000 0 f -4000 -8 c -6 -4 -2 0 2 4 6 8 B (T) d 2000 Vg=-1.8 V 120K 80K 40K 20K 10K 2K 1500 1000 -6 -4 -2 0 4 6 8 Vg=-2 V 1500 120K 80K 40K 20K 10K 2K 500 0 2 B (T) 1000 Rxy (Ω) 500 Rxy (Ω) -8 np (×1012 cm-2) -6000 -8000 1 Vg (V) -1.8 V: -2 V: μ μ n n 15 0.10 10 0.05 5 1 10 μp (m2V-1s-1) 8000 ns (×1012 cm-2) a 100 T (K) g 2.5 0 -1.8 V -2 V 2.0 -500 σn/σp -500 -1000 -1000 -1500 1.5 1.0 0.5 -1500 -2000 -8 -6 -4 -2 0 B (T) 2 4 6 8 -8 -6 -4 -2 0 2 4 6 8 B (T) 0.0 1 10 100 T (K) Figure S7 | Temperature- and gate-dependent hall resistance Rxy of ~50 nm-thick Cd3As2 thin film (sample Q1). a, Rxy under -1 V (gate voltage), indicative of electron-dominated n-type conductivity. b, Rxy under -1.5 V, showing a nonlinear behaviour originated from two-carrier transport owing to the gate-induced holes. c, Rxy under -1.8 V. The Cd3As2 channel undergoes a transition from electron- to holedominated transport as evidenced by the change of slope at B≥3T. d, Rxy under -2 V. The holes are dominant in Hall resistance. e, Gate-dependent sheet carrier density. It implies the ambipolar transport. The hole carrier density was extracted from the fits to the two-carrier transport model. Electron carrier density was obtained from the Hall effect measurements. The graduated background represents the amount and type of carriers, blue for holes and red for electrons. f, Temperature-dependent hole mobility (solid circles) and hole density (open squares) under -1.8 V (red) and -2 V (blue), obtained from the fits to the two-carrier transport model. g, Temperature-dependent conductance ratio σn/σp. The dashed line marks σn/σp=1. 7 a b 1500 Vg (V) 1.2x1013 Vg(V) 1000 p (cm-2) -0.8 -0.9 -1.05 -1.3 -2.2 Rxy (Ω) 500 -2.2 -1.3 -0.9 -0.8 12 9.0x10 6.0x1012 3.0x1012 1 10 0 100 T (K) c 800 μp (cm2V-1s-1) -500 -1000 600 400 Vg (V) -2.2 -1.3 -0.9 -0.8 200 -1500 0 -8 -6 -4 -2 0 2 4 6 8 1 10 100 T (K) B (T) Figure S8 | Two carrier transport of sample Q6. a, Rxy at 2 K under negative gate voltage. The black dash lines are the fitting curves of two-carrier model. b-c, Temperature-dependent hole mobility (b) and hole density (c) under negative gate voltage, obtained from the fits to the two-carrier transport model. 8 b 0.8 Vg = -0.5 V 0.6 2K 10 K 20 K 40 K 60 K 80 K 0.7 Vg = -0.9 V 0.6 △Rxx(B)/Rxx(0) △Rxx(B)/Rxx(0) a 0.4 0.2 2K 10 K 20 K 40 K 60 K 80 K 0.5 0.4 0.3 0.2 0.1 0.0 0.0 5.0x10-7 0.0 1.0x10-6 0 d c 3x10-7 4x10-7 5x10-7 Vg = -2.2 V 0.35 2K 10 K 20 K 40 K 60 K 80 K △Rxx(B)/Rxx(0) △Rxx(B)/Rxx(0) 0.40 Vg = -1.3 V 0.3 2x10-7 B2/Rxx(0)2 (T2Ω-2) B2/Rxx(0)2 (T2Ω-2) 0.4 1x10-7 0.2 0.1 2K 10 K 20 K 40 K 60 K 80 K 0.30 0.25 0.20 0.15 0.10 0.05 0.0 0.00 0.0 2.0x10-7 2 4.0x10-7 2 6.0x10-7 2 8.0x10-7 0.0 2.0x10-7 4.0x10-7 2 -7 -7 6.0x10 8.0x10 2 2 -2 1.0x10-6 B /Rxx(0) (T Ω ) -2 B /Rxx(0) (T Ω ) Figure S9 | The Kohler’s plots of the MR curves of sample Q6 at the gate voltage of -0.5 V (a), -0.9 V (b), -1.3 V(c), 0 V (d), -2.2 V (e), respectively. V. SdH oscillations analysis (sample Q2). Quantum lifetime could be obtained by the Dingle plot (Fig. S10a). With increasing carrier density, the quantum lifetime becomes smaller (Fig. 4e), suggesting the enhancement of the scattering process while the Fermi level is lifted into the conduction band. The cyclotron mobility μSdH consequently decreases from ~8000 cm2V-1s-1 to ~2000 cm2V-1s-1. At the same time, the quantum mobility μQ which is affected by both large and small angle scattering, could be estimate from μQ~1/Bstart (Bstart is the magnetic field where the first oscillation could be identified)1,5–7. The Bstart here increases with increasing gate voltage (Fig. S10b-f), leading to the decreasing of the μQ from about 3000 cm2V-1s-1 to 1500 cm2V-1s-1, which is comparable to the results calculated from the SdH oscillations and the measured Hall mobility (Fig. S10c). The amplitude of SdH oscillations decreases from ~15 to ~2 Ω, 9 indicating the declining of SdH oscillations. b 0 0.2 0.3 0.5 0.7 0.9 1.2 Ln[△RBsinh(λ)] 3 2 15 0 Vg=0.3 V 4K 8K 15K 30K 60K -10 1 0.20 10 Bstart 5 -5 0.16 -15 0.10 0.24 0.15 0.20 0.25 -1 0 1/B (T ) e 10 Vg=0.5 V -5 6K 10K 20K 40K 80K 0.30 Bstart 5 6K 10K 20K 40K -10 -15 0.35 0.15 0.20 4K 8K 15K 30K 60K 0.25 0.30 1/B (T-1) 1/B (T ) -1 d c 15 10 △R (Ω) Vg (V) 4 △R (Ω) a f 6 2 4 Bstart 0 Vg=0.7 V -5 4K 8K 15K 30K 60K -10 0.10 0.15 0.20 1/B (T-1) 6K 10K 20K 40K 80K 0.25 0.30 Bstart Bstart 2 △R (Ω) △R (Ω) △R (Ω) 5 0 Vg=0.9 V -2 4K 8K 15K 30K 60K -4 -6 0.15 0.20 6K 10K 20K 40K 80K 0.25 1 0 Vg=1.2 V 4K 8K 15K 30K 60K -1 -2 0.10 1/B (T-1) 0.15 6K 10K 20K 40K 80K 0.20 0.25 1/B (T-1) Figure S10 | SdH oscillations and Dingle plot (sample Q2). a, Dingle plots of ln[△ Rbsin(λ)] versus 1/B under different gate voltage. Lifetimes are obtained from the linear fit of the data. b-f, Temperature dependent SdH oscillations under the gate voltage of 0.3 V (b), 0.5 V (c), 0.7 V (d), 0.9 V (e) and 1.2 V (f) VI. Angular dependent transport measurements. Angular dependent transport measurements were carried out to probe the nature of SdH oscillations. The measurement configuration is shown in the inset of Fig. S11, where the sample normal is tilted away from the magnetic field by an angle θ. Within a small θ, the oscillations show aligned peaks and valleys, while in the large θ, oscillations starts to reduce. We believe that the compression of Fermi sphere in the reduced dimension of Cd3As2 causes such angular dependence of magnetoresistance. 10 60 θ B 50 △R (Ω) 40 30 Vg=0.9 V 60° 45° 30° 15° 10° 5° 0° 20 10 0 -9 -8 -7 -6 -5 -4 Bcosθ (T) -3 -2 Figure S11 | Angular dependence of SdH oscillations of sample Q1 at the gate voltage of 0.9 V. The SdH oscillations are plotted as a function of Bcosθ. The inset shows the measurement configuration. VII. Reproducibility of two-carrier transport from other Cd3As2 thin films. Except the sample mentioned in the main text, several other thin films were also measured with the ionic gating. All of them showed the gate-tunable SdH oscillations and two carrier transport, proving a good reproducibility of our results (Fig. S12-17). The related parameters obtained from SdH oscillations are summarized in Table SI. 11 a b 0V 1500 Vg -1.25V -1.5V -1.7V -1.95V -2.2V -2.5V 1.2x104 104 8x103 0.5 V Rxx (Ω) Rxx (Ω) 1000 1V 1.5 V 6x103 4x103 2V 500 2.5 V 2.9 V 3.2 V 0 100 0 200 100 200 T (K) T (K) Figure S12 | Gate-tunable Rxx-T curves of sample Q2. The results are similar to the main text results. a, Gate-induced insulator-metal transition was also observed under positive gate voltage. b, With negative gate voltages the Rxx-T curves show semiconducting-like feature. Also the curves cross over each other at about 80 K. 12 a b 6000 Vg=0V Vg=-1.25V 2000 4000 1000 Rxy (Ω) Rxy (Ω) 2000 0 0 -2000 T (K) -1000 1.9 -4000 -2000 10 -6000 -8 -6 -4 -2 0 2 4 6 8 -8 -6 -4 B (T) c 0 2 4 6 8 20 B (T) d Vg=-1.5V 1000 -2 30 Vg=-1.95V 1500 40 60 1000 500 Rxy (Ω) Rxy (Ω) 500 0 0 -500 -500 -1000 -1000 -1500 -8 -6 -4 -2 0 2 4 6 8 -8 B (T) -6 -4 -2 0 2 4 6 8 B (T) Figure S13 | Temperature-dependent hall resistance Rxy of ~50 nm-thick Cd3As2 thin film (sample Q2). a, The linear Rxy under zero gate voltage, indicative of electron-dominated n-type conductivity. b, Rxy under -1.25 V gate voltage showing a nonlinear behaviour originated from two-carrier transport owing to the gate-induced holes. c, Rxy under -1.5 V gate voltage. The Cd3As2 channel undergoes a transition from electron- to hole- dominated transport as evidenced by the change of slope at B≥4T. d, Rxy under -1.95 V. The holes are dominant in Hall resistance. 13 a c -1.5V -1.7V -1.95V 6 σp/σn 5 4 3 2 1 10 20 30 μp (cm2V-1s-1) d b 40 50 60 70 80 T (K) 600 500 400 -1.5V -1.7V -1.95V 300 0 10 20 e 40 50 60 40 50 60 T (K) 8 np (x1012 cm-2) 30 -1.5V -1.7V -1.95V 7 6 5 4 3 0 10 20 30 T (K) Figure S14 | Temperature- and gate-dependent carrier density and mobility (sample Q2). a, Gate-dependent sheet carrier density. It implies the ambipolar transport. The hole carrier density was extracted from the fits to the two-carrier transport model. Electron carrier density was obtained from the Hall effect measurements. b, Gate-dependent mobility of holes and electrons. The insets sketch the positions of the Fermi level. The graduated background in a and b represents the amount and type of carriers (blue for holes and red for electrons). c-e, Temperature-dependent conductivity ratio (c), hole mobility (d) and hole density (e), obtained from the fits to the two-carrier transport model. Dashed lines in c, as guides to the eye, display the temperature trends of the conductivity ratio. 14 V1=gV 2 0 -2 0 d 20 Q3 Vg=0V 10 △R (Ω) 2 R (Ω) R (Ω) 4 c Q2 Vg=0.75V 4 Q2 Vg=0.5V 6 6 0 -2 T (K) 0 -4 -4 -6 0.20 -6 0.10 0.25 0.15 0.20 0.5V Q2 T=2K 0.20 1/B (T-1) 0.25 Q3 0.9 Vg=0V 0.8 Vg=0.5V 0.7 0.6 0 5 10 15 0.15 20 25 0.20 0.25 1/B (T ) h 7.5 Ln[△R/R·Bsinh(λ)] 0.75V 0.10 -1 g 1.0 △σxx(T)/△σxx(0) R (Ω) 1V 0.25 1/B (T ) f 1.25V 0.20 -1 Q3 Q2 0.5V Q2 0.75V Q3 0V Q3 0.5V 0.20 7.0 6.5 Vg=0V 6.0 5.5 0.15 0.10 5.0 4.0 0.15 0.18 1/B (T-1) T (K) 4 6 8 10 15 20 0.05 Vg=0.5V 4.5 2.5 R e 0.15 0.15 1/B (T ) 1/B (T-1) 5Ω -20 0.10 0.25 -1 1/B (T-1) 0.15 2 xx K2 K5.2 K4 K6 K8 K01 K51 K02 -2 -6 0.10 2 -10 -4 -8 0.10 Q3 Vg=0.5V 4 △R (Ω) b 8 ).u.a( a 0.21 0 1 2 3 4 5 6 Landau Index n 8 6 4 2 0 2- 4- 6- 8Figure S15 | SdH oscillations of Cd3As2 thin films. a-b, Temperature-dependent )T( dleiF citengaM amplitude of the SdH oscillations at 0.5 and 0.75 V (sample Q2), respectively. c-d, Temperature-dependent amplitude of SdH oscillations (sample Q3) at 0 and 0.5 V, respectively. e, Gate-dependent amplitude of the SdH oscillations (Q2) at 2 K. f, Normalized conductivity amplitude versus temperature for sample Q3 at gate voltage of 0 and 0.5 V. g, Dingle plot at 2 K of sample Q3 at different gate voltage of 0 and 0.5 V. h, Landau level index n with respect to 1/B of sample Q2 and Q3 under different gate voltage. Integer indices denote the △Rxx peak positions in 1/B and half integer indices represent the △Rxx valley positions. The intercepts are close to 0.5. 15 3000 Vg=-1.25V 2000 Rxy (Ω) b 2K 2.5K 4K 6K 8K 10K 1000 0 Vg=-1.5V 800 2K 10K 20K 30K 40K 60K 400 Rxy (Ω) a -1000 0 -400 -2000 -800 -3000 -10 -8 -6 -4 -2 0 2 4 6 8 10 -10 -8 Magnetic Field (T) Vg=-1.7V 600 d 2K 10K 20K 30K 40K 60K 400 Rxy (Ω) -4 -2 0 2 4 6 8 10 Magnetic Field (T) 200 600 Vg=-1.95V 2K 10K 20K 30K 40K 60K 400 Rxy (Ω) c -6 0 -200 200 0 -200 -400 -400 -600 -10 -8 -6 -4 -2 0 2 4 6 8 -600 10 Magnetic Field (T) -10 -8 -6 -4 -2 0 2 4 6 8 10 Magnetic Field (T) Figure S16 | Temperature-dependent Hall resistance Rxy of sample Q4. Two-carrier transport was also observed in sample Q4. When scanning the gate voltage to reach the negative range, the hole-dominated transport takes place, showing a good reproducibility of ionic gating on different MBE-grown samples. 16 6 Q6 △Rxx (Ω) 4 2 0 Vg = 0 V -2 3K 6K 10 K 20 K 40 K -4 -6 0.10 0.15 0.20 0.25 2K 4K 8K 15 K 30 K 60 K 0.30 B (T) Figure S17 | SdH oscillations of Cd3As2 thin films (sample Q6). VIII. Band evolution of Cd3As2 thin films According to our calculation results, at a thickness of ~ 50 nm the bulk Dirac cone is fully gapped, with bulk gap larger than 20 meV. This gap falls off with increasing thickness, and is very close to zero for a thin film of thickness ~ 60 nm. This variation in the bulk gap is in reasonable agreement with our experimental results. Since Cd3As2 also has an inverted gap, apart from the bulk Dirac point, it also exhibits surface Dirac crossings when confined in a quantum well geometry. These surface cones are highlighted in red in Figure S18b and c. Note that in contrast to the bulk cone, the surface crossing is already gapless for films as thin as ~12 nm. This behavior is similar to the case of Na3Bi, the other putative three-dimensional Dirac 17 semimetal8. Figure S18 | Band evolution of Cd3As2 thin films. (a) Brillouin zone for the P42/nmc unit cell used for the first-principles-derived tight-binding computations. Band structures for slabs with representative thicknesses (b) 8 nm and (c) 12 nm are shown, with the bulk bands shaded in blue. The surface bands are highlighted in red. (d) Variation of the bulk band gap, Ebulk, with increasing thickness of the slab. Table SI| Estimated parameters from the SdH oscillations at T=2K sample Vg(V) FSdH(T) kf(Å) mcyc(me) vF(105 m/s) Ef(meV) t(10-13 s) l(nm) μSdH(cm2V-1s-1) Q2 0.75 29.31 0.0298 0.046 7.5 148 1.57 118 6021 Q3 0 22.96 0.0264 0.030 10 176 0.86 87 4995 Q3 0.5 27.92 0.0291 0.035 9.7 186 1.08 105 5450 18 References 1. Cui, X. et al. 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