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Subscriber access provided by INDIAN INST OF SCI EDUC & RES Nano Letters is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties. Communication Surface-dominated Conduction in a 6 nm-thick Bi2Se3 Thin Film Liang He, Faxian Xiu, Xinxin Yu, Marcus Teague, Wanjun Jiang, Yabin Fan, Xufeng Kou, Murong Lang, Yong Wang, Guan Huang, Nai-Chang Yeh, and Kang L. Wang Nano Lett., Just Accepted Manuscript • DOI: 10.1021/nl204234j • Publication Date (Web): 08 Feb 2012 Downloaded from http://pubs.acs.org on February 14, 2012 Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.

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Liang He, Faxian Xiu, Xinxin Yu, Marcus Teague, Wanjun Jiang, Yabin Fan, Xufeng Kou, Murong Lang, Yong Wang, Guan Huang, Nai-Chang Yeh, and Kang L. Wang Nano Lett., Just Accepted Manuscript • DOI: 10.1021/nl204234j • Publication Date (Web): 08 Feb 2012 Downloaded from http://pubs.acs.org on February 14, 2012 Just Accepted Subscriber access provided by INDIAN INST OF SCI EDUC & RES

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Page 1: Surface-dominated Conduction in a 6 nm-thick Bi2Se3 Thin Film IMP

Subscriber access provided by INDIAN INST OF SCI EDUC & RES

Nano Letters is published by the American Chemical Society. 1155 Sixteenth StreetN.W., Washington, DC 20036Published by American Chemical Society. Copyright © American Chemical Society.However, no copyright claim is made to original U.S. Government works, or worksproduced by employees of any Commonwealth realm Crown government in the courseof their duties.

Communication

Surface-dominated Conduction in a 6 nm-thick Bi2Se3 Thin FilmLiang He, Faxian Xiu, Xinxin Yu, Marcus Teague, Wanjun Jiang, Yabin Fan, XufengKou, Murong Lang, Yong Wang, Guan Huang, Nai-Chang Yeh, and Kang L. Wang

Nano Lett., Just Accepted Manuscript • DOI: 10.1021/nl204234j • Publication Date (Web): 08 Feb 2012

Downloaded from http://pubs.acs.org on February 14, 2012

Just Accepted

“Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are postedonline prior to technical editing, formatting for publication and author proofing. The American ChemicalSociety provides “Just Accepted” as a free service to the research community to expedite thedissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscriptsappear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have beenfully peer reviewed, but should not be considered the official version of record. They are accessible to allreaders and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offeredto authors. Therefore, the “Just Accepted” Web site may not include all articles that will be publishedin the journal. After a manuscript is technically edited and formatted, it will be removed from the “JustAccepted” Web site and published as an ASAP article. Note that technical editing may introduce minorchanges to the manuscript text and/or graphics which could affect content, and all legal disclaimersand ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errorsor consequences arising from the use of information contained in these “Just Accepted” manuscripts.

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Surface-dominated Conduction in a 6 nm-thick

Bi2Se3 Thin Film

Liang He1*

, Faxian Xiu2, Xinxin Yu

1, Marcus Teague

4,Wanjun Jiang

1, Yabin Fan

1, Xufeng Kou

1,

Murong Lang1, Yong Wang

3, Guan Huang

1, Nai-Chang Yeh

4, Kang L. Wang

1*.

1Device Research Laboratory, Department of Electrical Engineering, University of California, Los

Angeles, California, 90095, USA 2 Department of Electrical and Computer Engineering, Iowa State

University, Ames, 50011, USA 3 State Key Laboratory of Silicon Materials and Center for Electron

Microscopy, Department of Materials Science and Engineering, Zhejiang University, Hangzhou,

310027, China, 4Department of Physics, California Institute of Technology, Pasadena, California,

91125, USA

*To whom correspondence should be addressed. E-mail: [email protected], [email protected],

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Abstract

We report a direct observation of surface dominated conduction in an intrinsic Bi2Se3 thin film with a

thickness of 6 quintuple layers (QLs) grown on lattice-matched CdS (0001) substrates by molecular

beam epitaxy (MBE). Shubnikov-de Haas (SdH) oscillations from the topological surface states suggest

that the Fermi level falls inside the bulk band gap and is 53 ± 5 meV above the Dirac point, in

agreement with 70 ± 20 meV obtained from scanning tunneling spectroscopies (STS). Our results

demonstrate a great potential of producing genuine topological insulator devices using Dirac Fermions

of the surface states, when the film thickness is pushed to nano-meter range.

Keywords: Intrinsic topological insulator, Bi2Se3, transport properties, surface states, Quantum

oscillations.

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ToC figure

0.8

0.7

0.6

0.5

0.4

0.3

dI/dV (a.u.)

-400 -300 -200 -100 0 100 200

E (meV)

-30

-20

-10

0

10

20

30

∆∆ ∆∆Rxx (

ΩΩ ΩΩ)

0.300.250.200.15

1/B (T-1)

1.9 K 5 K 8 K 10 K

Dirac point

Intrinsic 3D topological insulators of Bi2Se3 have been grown on CdS (0001) substrates by molecular

beam epitaxy. Shubnikov-de Haas (SdH) oscillations and scanning tunneling spectroscopies confirm the

Fermi level is within the bulk band gap. Our results demonstrate a great potential of producing genuine

topological insulator devices using Dirac Fermions of the surface states.

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Three-dimensional (3D) topological insulators (TIs) have attracted great attention from both

theoretical and experimental aspects1-6. It is known that they have a semiconductor gap in the bulk with

an odd number of Dirac-cone surface states. Soon after theoretical predictions, the surface states of 3D

TIs have been demonstrated by angle-resolved photoemission spectroscopy (ARPES)7-10 and scanning

tunneling microscopy (STM)9, 11, 12. However, a direct transport measurement of the surface effects is

significantly hindered by the dominant bulk carrier conduction. Scientist have tried various approaches

to overcome the bulk conduction, such as electrical tuning of the Fermi level into bulk band13, 14, counter

doping with Ca or Na15, and synthesizing novel complex materials such as (BiSb)2Se316, and

Bi2(SeTe)317, 18. To some extent, these approaches have demonstrated success in enhancing surface

conduction. However, the fundamental understanding of surface conduction in high quality samples is

crucial for utilization of surface states in microelectronics and spintronics. In this paper, we report high-

crystalline quality Bi2Se3 thin films grown on CdS (0001) substrate by molecular beam epitaxy

demonstrate surface-dominated conduction. Importantly, the Fermi levels of current thin films fall

inside the bulk band gap. As a result, the surface state conduction can be clearly distinguished from

other conducting channels. In particular, for a 6 QLs thin film, we show most of conduction come from

the surface.

Bi2Se3 thin films were grown with an ultra-high vacuum MBE chamber on lattice-matched insulating

CdS (0001).19 After growth, standard Hall bar devices were fabricated with a physical mask, as shown

schematically in Fig. 1 (a). The longitudinal sheet resistance (Rs) as a function of temperature (T) is

displayed in Fig. 1 (b), where four different regimes can be clearly identified, marked as I, II, III and IV

from high to low temperatures. In regime I, for thinner films (< 9 QLs), Rs exponentially increases as

the temperature decreases. This is most likely associated with the bulk band gap. The activation energy

of it can be estimated from the Arrhenius slope of ln(Rs) vs. 1/T .20, 21 The thickness dependent

activation energy is plotted in Fig. 1 (c). The systematic increase of the estimated bulk band gap with

the reduced the film thickness is attributed to the quantum confinement of the film along the growth

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direction (perpendicular to the substrate), which is qualitatively agreed with the recent ARPES

measurements of Bi2Se3 grown on SiC (0001) by MBE.22 For thicker films, however, Rs does not show

the same exponential behavior at high temperatures, which can be ascribed to the overwhelming

electrons activated from the bulk impurity band as will be discussed later.

In Regime II, the resistance reduces as temperature decreases, resembling a metallic behavior as

observed widely in TIs.13, 16, 24 Such a decrease can be explained by alleviated phonon scatterings when

temperature decreases. This can be further confirmed by a power-law increase of mobility ( 2Tµ −∝ ), as

will be described in Fig. 2 (e) (dashed line). In Regime III (30 K < T < ~ 80 K), the resistivity exhibits

another exponential increase with respect to 1/T. This exponential increase is most likely associated

with the frozen-out effect of electrons from the bulk conduction band to a shallow impurity band below

it.21, 25 In Regime IV (T < 30 K), the resistivities of all samples approach to constant values. A similar

temperature-dependent behavior was reported in our previous work: Bi2Se3 grown on Si (111)

substrate.26 And this temperature regime is believed to be dominated by surface conduction.

In Region IV where the bulk carriers freeze out, the transport is presumably a combination of surface

states and impurity band conduction.17, 18, 21 The sheet conductance is monotonically increases with film

thickness as shown in Fig. 1(d). This variation of the conductance with film thickness is attributed to the

impurity band. By fitting the conductance of thicker films (20 to 60 QLs), where the impurity band

conduction dominates, a linear relationship of G = 8.75 × (t-6.4) can be obtained (solid line in Fig. 1 (d)

and (e)), where G is the conductance in the unit of e2/h, and t is the film thickness. This result suggests

that below a critical thickness 6.4 QLs, the contribution from the thickness dependent component is

close to zero.

We have noticed linearly fitted solid line from the thicker samples deviated from the data of thinner

films below 10 QLs, as shown in Fig. 1 (e). The difference of ~10 e2/h, as indicated by the double

arrows, is considered to be the conduction from the surface states which agrees closely with the Hall

data to be described later. As samples getting thinner, the surface states also open a band gap because of

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the hybridization between the top and bottom surfaces;22 therefore the metallic surface states seem to

disappear. These samples behave like normal insulators and thus the conductance drops dramatically

down to 1.5 e2/h (5 QLs) and 0.1 e2

/h (3 QLs). Based on the simplified model, for samples around the

critical thickness (~ 6.4 QLs), the surface state conduction is the dominant channel. In other words, for

our 6 QL sample, most of the total conduction is provided by surface states.

In order to further investigate the multiple channel conduction for thicker films, magnetic field

and temperature dependent longitudinal resistance (Rxx) and Hall resistance (Rxy) have been measured.

These data reveal the co-existence of three conducting channels: the bulk, the impurity band and the

surface states.17 The parallel Hall conductance is given by

SurfacepurityBulk

Sxy

xy

xy GGGRR

RG ++=

+≡ Im22

(1)

where Rxy is the Hall resistance, Rs is the sheet resistance, GBulk, Gimpurity and Gsurface represent the Hall

conductance of the bulk, the impurity band, and the surface states, respectively. Additionally, the Hall

conductance of each channel is described by a semiclassical expression,

( )221 B

BenG

µ

µµ

+×= , (2)

where n is the 2D carrier density and µ is the mobility of each channel.16 As an example, we present

the analysis results of the Hall conductance for a 10 QL sample at different temperatures as described

below.

At high temperatures (Regime II in Fig. 1 (b)) where the phonon scattering dominates, the total

conductance is then overwhelmed by electrons in the bulk conduction band excited from the impurity

band. As a result, the total conductance of Gxy can be simplified by the dominant bulk conducting

channel, as given in Fig. 2 (a). At low temperature (Regime IV in Fig. 1(b)), when all electrons are

frozen in the impurity band, there is nearly no contribution from bulk, thus the total conduction is a

combination of those of the surface and the impurity band, evident in Figure 2 (b). In the intermediate

temperature (Regime III in Fig. 1(b)), the total conduction consequently results from all three channels,

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illustrated in Fig. 2 (c). Following this procedure, we can obtain the temperature dependence of carrier

density and mobility for the three channels (1.9 to 300K).

Figure 2(d) illustrates the temperature dependence of the two-dimensional carrier density of the three

channels. The bulk carrier densities (green triangles) decrease exponentially as carriers are frozen to the

impurity band. Since the carriers in the bulk conduction band are electrons, their temperature dependent

density can be described as a classic Fermi-Dirac distribution of ( )1/ /0 +=

TkE

bBaenn (solid yellow line

in Fig. 2 (d)), where n0 is the bulk carrier density of ~ 4 × 1015 cm-2, and Ea of 20 meV is the energy gap

between the impurity band and the bottom of the bulk conduction band. The carrier densities of the

impurity band (blue squares) and surface states (red circles) remain approximately a constant of 1.3 ×

1013 cm-2 and 4 × 1011 cm-2, respectively. Figure 2 (e) shows the corresponding mobility at different

temperatures. The mobility of bulk electrons (green triangles) exhibits a power law µ ∝ T-2 at high

temperatures, consistent with the dominant phonon scattering as mentioned before in the Region II of

Fig. 1 (b). At low temperatures (T < 20 K), mobilities of both the impurity band and the surface states

reach constant values of ~ 380 cm2/V⋅s and ~ 5000 cm2/V⋅s, respectively. Based on the above analysis,

we can subsequently estimate the longitudinal conductance Gxx (=neu) of 20 e2/h and 8 e2/h for the

impurity band and the surface states, respectively. The numbers are in quantitative agreement with the

previous results from the thickness dependent conductance as shown in Fig. 1 (e), in which the

estimated conductance of the impurity band and surface states is 22 e2/h and 10 e2/h respectively for 10

QL sample.

As we demonstrated above, samples with a film thickness around 6.4 QLs will have the most

pronounced surface conduction. Indeed, we have observed characteristic quantum oscillations originated

from the surface states for our 6 QLs sample. In Fig. 3 (a), we present the field dependent longitudinal

resistance, Rxx, acquired at 1.9K for the 6 QL sample. Strong oscillations of Rxx at various temperatures

after subtracting a smooth background can be observed, as shown in Fig. 3 (b). The oscillations become

stronger with the increase of magnetic field and decrease of temperature. For a two-dimensional Fermi

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surface, the peak positions depend only on the field )cos(θBB =⊥ , normal to sample surface, (θ is the

tilt angle between B and c). As show in the inset of Fig. 3 (b), the peak field of Landau level n=3.5

(second peak in Fig. 3(a)) has been plotted at different field angels. It follows 1/cos(θ) perfectly,

suggesting the SdH oscillations originated from a 2D Fermi surface. It is well know that in the SdH

oscillations, the Landau level index n is related to the cross section area of the Fermi surface (SF) by

eBSn F

h=+ )(2 γπ , (3)

where e is the electron charge, ћ is the Plank’s constant divided by 2π, B is the magnetic flux density,

and γ = 1/2 or 0 represent the Berry phase of π or 0. As shown in Fig. 3 (c), the value of 1/B

corresponding to the maximum and the minimum in ∆Rxx (arrows in Fig. 3(a) and lines in Fig. 3(b)) is

plotted as a function of the Landau-level number. A linear fit yields SF = 1.53 × 1017 m-2, with the Fermi

wave vector kF = 0.022 Å-1, and a 2D carrier density of 3.9 × 1011 cm-2, consistent with our previous

results of 4 × 1011 cm-2 for the surface states in Fig. 2 (d). The n-axis intercept, γ ~ 0.35 ± 0.08 slightly

deviates from exactly π Berry phase, as has also been reported on other SdH studies of TIs.17, 18, 24, 27

Following the Lifshitz-Kosevich (LK) theory,28 the temperature dependence of the SdH amplitude is

described by ( ) / (0) ( ) / sinh( ( ))xx xxT T Tσ σ λ λ∆ ∆ = . The thermal factor is given by

)/(2)( 2 eBTmkT cycB hπλ = , where mcyc is cyclotron mass and ћ is the reduced Planck constant. As shown

in Fig. 3 (d), the best fit gives the cyclotron mass mcyc = 0.07 me, where me is the free electron mass.

Assuming that the electrons are Dirac type, the Fermi velocity can be calculated

as smmk cycFF /106.3/ 5×== hν , and meVmE FcycF 532 == ν . The estimated Fermi level of 53 meV

above the Dirac point is surprisingly low, suggesting the surface carriers are electrons and the EF is

within the bulk band gap.

To acquire the lifetime of the surface states (τ ), the Dingle factor De− has been examined, where

2 22 / ( )F FD E eBVπ τ=13, 16. Note that /R R∆ is proportional to [ ( ) / sinh( ( ))] DT T eλ λ − , and the lifetime

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can be inferred from the slope in the logarithmic plot of

2 20log[( / ) sinh( ( ))] ~ [2 / ( )] (1 / )F FR R B T E eV Bλ π τ∆ × (Fig. 3 (e)). By applying the extracted cyclotron

mass, the scattering time τ = 1.3 × 10-12 s can be estimated. Thus the mean-free path of the surface

electrons is mF

7106.4 −×== τνl , and the surface mobility is sVcmm

e

cyc

⋅== /200,13 2τµ . We have

noticed that the estimated mobility is higher than the results from our previous fitting from Hall data of

surface carrier mobility, 5000 cm2/Vs. In other systems,17, 28, 29 the similar discrepancy was also

observed, and the reason maybe lies in the difference between relaxation time and scattering time.30

To investigate the surface states as well as the position of surface Fermi level, we performed ARPES

measurements on our samples. Figure 4(a) presents a standard ARPES spectroscopy cut along Γ - K

direction of a 60 QL sample, the zero point of the energy scale has been shifted to the Dirac point. We

have noticed that the Fermi level of the ARPES data is inside the bulk conduction band. This may be

due to the n-type doping over long time between sample growth and ARPES measurement, as

previously show 18, 31. Another possible reason is due to optical doping induced charge accumulation

during ARPES measurement.31 By finding the maximum of the surface state in the K direction for

different energies, we can attain the Fermi area and the surface carrier density (ns) as a function of

energy. In Figure 4 (b), the horizontal axis has been scaled to fit our experiment data (red circle). The

green square is adopted from Ref. 24 and the purple triangles are the results from our other samples of

Bi2Se3 grown on Si (111).32 The consistence between transport results and ARPES supports our

estimation of the Fermi level position.

Scanning tunneling spectroscopy (dI/dV) was also performed on the 6 QL sample to measure the

density of states (DOS). As expected, the minimum of the conduction corresponding to the Dirac point

is ~ 70 ± 20 meV below the Fermi level (Fig. 4(c)), in reasonable agreement with our estimation from

the SdH oscillations. The STS data further confirms that our Fermi level is inside the bulk band gap and

very close to the Dirac point.

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To conclude, we have observed surface dominated conduction from a 6 QL Bi2Se3 thin film grown by

MBE. We demonstrated that the intrinsic Bi2Se3 thin film has a Fermi level positioned within bulk band

gap. Our results shed the light on the possibility of producing genuine topological insulator states on

lattice-matched CdS substrate, and pave a pathway towards the practical device application of

topological insulators.

Acknowledgements This work was in part supported by the Focus Center Research Program - Center

on Functional Engineered Nano Architectonics (FENA) and DARPA. Y. W. acknowledges the support

from the National Science Foundation of China (No. 11174244).

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(4), 042112-3. 16. Qu, D.-X.; Hor, Y. S.; Xiong, J.; Cava, R. J.; Ong, N. P. Science 2010, 329, (5993), 821-824. 17. Ren, Z.; Taskin, A. A.; Sasaki, S.; Segawa, K.; Ando, Y. Physical Review B 2010, 82, (24), 241306. 18. Taskin, A. A.; Ren, Z.; Sasaki, S.; Segawa, K.; Ando, Y. Physical Review Letters 2011, 107, (1), 016801. 19. Kou, X. F.; He, L.; Xiu, F. X.; Lang, M. R.; Liao, Z. M.; Wang, Y.; Fedorov, A. V.; Yu, X. X.; Tang, J. S.; Huang, G.; Jiang, X. W.; Zhu, J. F.; Zou, J.; Wang, K. L. Applied Physics Letters 2011, 98, 242102. 20. Grove, A. S., Physics and Technology of Semiconductor Devices. Wiley: 1967. 21. Köhler, H.; Fabbicius, A. physica status solidi (b) 1975, 71, (2), 487-496. 22. Zhang, Y.; He, K.; Chang, C.-Z.; Song, C.-L.; Wang, L.-L.; Chen, X.; Jia, J.-F.; Fang, Z.; Dai, X.; Shan, W.-Y.; Shen, S.-Q.; Niu, Q.; Qi, X.-L.; Zhang, S.-C.; Ma, X.-C.; Xue, Q.-K. Nature Physics

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Physics 2010, 6, (12), 960-964. 25. Kulbachinskii, V. A.; Miura, N.; Nakagawa, H.; Arimoto, H.; Ikaida, T.; Lostak, P.; Drasar, C. Physical Review B 1999, 59, (24), 15733. 26. He, L.; Xiu, F.; Wang, Y.; Fedorov, A. V.; Huang, G.; Kou, X.; Lang, M.; Beyermann, W. P.; Zou, J.; Wang, K. L. Journal of Applied Physics 2011, 109, 103702. 27. Brüne, C.; Liu, C. X.; Novik, E. G.; Hankiewicz, E. M.; Buhmann, H.; Chen, Y. L.; Qi, X. L.; Shen, Z. X.; Zhang, S. C.; Molenkamp, L. W. Physical Review Letters 2011, 106, (12), 126803. 28. Shoenberg, D., Magnetic Oscillations in Metals. Cambridge University Press, Cambridge: 1984. 29. Eto, K.; Ren, Z.; Taskin, A. A.; Segawa, K.; Ando, Y. Physical Review B 2010, 81, (19), 195309. 30. Das Sarma, S.; Stern, F. Physical Review B (Condensed Matter and Materials Physics) 1985, 32, (12), 8442. 31. Li, Y.-Y.; Wang, G.; Zhu, X.-G.; Liu, M.-H.; Ye, C.; Chen, X.; Wang, Y.-Y.; He, K.; Wang, L.-L.; Ma, X.-C.; Zhang, H.-J.; Dai, X.; Fang, Z.; Xie, X.-C.; Liu, Y.; Qi, X.-L.; Jia, J.-F.; Zhang, S.-C.; Xue, Q.-K. Advanced Materials 2010, 22, (36), 4002-4007. 32. Lang, M.; He, l.; Xiu, F.; Yu, X.; Tang, J.; Wang, Y.; Kou, X.; Jiang, W.; Chang, L.-T.; Fan, Y.; Jiang, X.; Wang, K. L. Acs Nano, 2012, in-print.

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12

Figure captions

Figure 1. (color online). (a) Schematic diagram of a typical Hall bar sample. The channel size is 8mm ×

1mm. A constant current geometry was used for transport measurement. (b) Temperature dependent

sheet resistance Rs (Rxx) of films ranging from 5 to 60 QLs. (c) Estimated bulk band gap vs. film

thickness. (d) Total conductance vs. film thickness at 5 K. The solid line presents a linear fit for the four

thicker films (20 to 60 QLs), exhibiting a thickness dependence of impurity band conduction and

enabling the determination of a critical thickness of 6.4 QL (intercepting the abscissa), below which

surface states is the only conducting channel at low temperature. (e) Expanded plot for the thin film

range of (d), dotted square. The solid line is the same solid line in (d). The dashed line is the fitted data

for thin layer samples. The difference representing the surface conduction fit to 6.4 QL sample is ~ 10

e2/h.

Figure 2 (color online). Hall conductance of a 10 QL sample, from which transport properties of three

channels: the bulk, the impurity band and the surface states at various temperatures have been extracted.

Magnet field dependent Gxy at various temperatures of (a) 220 K, (b) 20 K and (c) 40 K. Open circles

are experimental data and solid lines are fitted results (d) 2D carrier density vs. temperature. Solid

yellow line represents the Fermi-Dirac distribution of the bulk carrier density equivalent to 2D. (e)

Mobility vs. temperature for the three channels. Dashed line represents the power low dependence of µ

∝ T -2, which suggests the mechanism of phonon scattering in these temperatures.

Figure 3 (color online). Shubnikov-de Haas oscillations of the surface states of a 6 QL sample. (a)

Longitudinal resistance Rxx vs. magnetic field at T = 1.9 K. Solid arrows indicate the integer Landau

levels from the valley values; open arrows give the peak values. (b) ∆Rxx vs. 1/B at different

temperatures. The insert shows the field position of the n= 3.5 LL peak varies with θ as 1/cosθ (solid

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13

black line), suggesting a 2D Fermi surface. (c) Landau level index plot: 1/B vs. n. The open (close)

circles are the Landau level of the maxima (minima) of ∆Rxx. (d) Normalized conductivity amplitude

∆σxx(T)/∆σxx(0) vs. temperature ( 7.6 T). The effective mass deduced is ~ 0.07 me. (e) Dingle plot of

ln[(∆R/R0)Bsinh(λ)] vs. 1/B, used to determine τ and l .

Figure 4 (color online) (a) A standard APRES image of a 60 QL sample showing the surface states and

the Dirac point. (b) Surface density of states (ns) vs. Energy. The data are extracted from ARPES

measurement, and horizontal axis has been scaled to fit the transport measurements. The red circle

indicates our experiment result in this paper. The green square is adopted from Ref. 24. The purple

triangles are the data from our other samples of Bi2Se3 grown on Si (111).32 (c) Scanning tunneling

spectroscopy of a 6 QL sample. Spatially averaged density of states (dI/dV) measurements show the

Dirac point is about ~ 70 ± 20 meV below the Fermi surface.

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14

Figure 1

100

101

102

103

104

105

Rs (

ΩΩ ΩΩ/ )

4003002001000

T (K)

10 QL20 QL

5 QL

8 QL

9 QL

6 QL

60 QL

I

CdS

Vxx

Vxy(a) (b)

Fig. 1

T = 5 K

B

(c) (e)(d)T = 5 K

IV III II I

[21]

1.0

0.8

0.6

0.4

0.2

0.0

Eg (eV)

108642t (QL)

This paper Zhang etc. [24]

400

300

200

100

0

Gs (e2/h)

605040302010t (QL)

40

30

20

10

0

Gs (e2/h)

12108642t (QL)

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15

Figure 2

2

4

103

2

4

104

2

µµ µµ (cm

2/Vs)

2 4 6 8

102 4 6 8

1002

T (K)

Surface States Impurity Band Bulk

1011

1012

1013

1014

1015

n2D (cm

-2)

2 4 6 8

102 4 6 8

1002

T (K)

Surface States Impurity Band Bulk

-60

-40

-20

0

20

40

60

Gxy (mS)

-8 -4 0 4 8B (T)

T = 220 K

Exp Fitted

-200

-100

0

100

200

Gxy (

µµ µµS)

-8 -4 0 4 8B (T)

Exp Fitted Surface Impurity Band

T = 20 K

-20

-10

0

10

20

Gxy (mS)

-8 -4 0 4 8B (T)

Exp Fitted Bulk Surface Impurity Band

T = 40 K

µµµµ ∝∝∝∝ T -2.0

Fig. 2

(a)

(d) (e)

(c)(b)

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16

Figure 3

20.70

20.65

20.60

20.55

20.50

Rxx (k

ΩΩ ΩΩ)

9876543

B (T)

-40

-20

0

20

∆∆ ∆∆Rxx (

ΩΩ ΩΩ)

0.300.250.200.15

1/B (T-1)

1.9 K 5 K 8 K 10 K

(a) (b)

(c) (d)

Fig. 3

(e)

2.53.5

4.5

3

4

T = 1.9 K

0.30

0.25

0.20

0.15

0.10

0.05

0.00

1/B (T-1)

543210

n

1.0

0.9

0.8

0.7

∆σ

∆σ

∆σ

∆σxx (T) / σσ σσ

xx (0)

1086420

T (K)

-6.5

-6.0

-5.5

-5.0

-4.5

-4.0

Ln [

∆∆ ∆∆R/R

0Bsinh( λλ λλ)]

0.200.12

1/B (T-1)

1.9 K

5 K

8 K

10 K

10

8

6n=3.5 H (T)

6040200

Angle θθθθ (deg)

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17

Figure 4

150

100

50

0

-50

-100

E - E

D (meV)

43210ns (10

12cm

-2)

This paper Analytis etc. [21] Lang etc. [28]

0.8

0.7

0.6

0.5

0.4

0.3

dI/dV (a.u.)

-400 -300 -200 -100 0 100 200

E (meV)

200

-50

0

50

100

150

E-E

D(meV)

(a)

0.0-0.8 0.8K//(Å

-1)

Fig. 4

(b) (c)300

250

Dirac point

[24][32]

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Page 19: Surface-dominated Conduction in a 6 nm-thick Bi2Se3 Thin Film IMP

105I(b) IV III II I

103

104

/

)

5 QL

8 QL

9 QL

6 QLVxy

(a) (b) IV III II I

101

102

Rs (

10 QL 20 QL

9 QL

60 QLCdS

VxxB

1 0 400 40

100

4003002001000T (K)

60 QLCdS

( ) ( )(d)1.0

0.8

0 6V)

This paper Zhang etc. [20]

400

300h)

40

30

h)

T = 5 K

(c) (e)(d)T = 5 K[22]

0.6

0.4

0 2

E g (e

V

200

100

Gs (

e2 /

20

10

Gs (

e2 /

0.2

0.0108642

t (QL)

0605040302010

t (QL)

012108642

t (QL)t (QL) t (QL) t (QL)Fig. 1

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Page 20: Surface-dominated Conduction in a 6 nm-thick Bi2Se3 Thin Film IMP

-60

-40

-20

0

20

40

60

Gxy (mS)

-8 -4 0 4 8B (T)

T = 220 K

Exp

Fitted

-200

-100

0

100

200

Gxy (µµ µµS)

-8 -4 0 4 8B (T)

Exp

Fitted Surface Impurity Band

T = 20 K

-20

-10

0

10

20

Gxy (mS)

-8 -4 0 4 8B (T)

Exp

Fitted Bulk Surface Impurity Band

T = 40 K

(a)

(d) (e)

(c)(b)

2

4

103

2

4

104

2

µµ µµ (cm2/Vs)

2 4 6 8

102 4 6 8

1002

T (K)

Surface States

Impurity Band

Bulk

1011

1012

1013

1014

1015

n2D (cm-2)

2 4 6 8

102 4 6 8

1002

T (K)

Surface States

Impurity Band

Bulk

µµµµ ∝∝∝∝ T -2.0

Fig. 2

(d) (e)

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20.7020

(a) (b)

20.65

20 60x (k

) 0

20

xx (

)2.53.5 3

420.60

20.55

Rxx

-40

-20R

x

1.9 K 5 K 8 K 10 K

4.5 T = 1.9 K10

8

6n=3.

5 H

(T)

6040200

20.509876543

B (T)0.300.250.200.15

1/B (T-1)

( ) (d) ( )0.30 -4.0

6040200Angle (deg)

(c) (d) (e)0.30

0.25

0.20

-1)

1.0

0.9 xx (

0)

-5 0

-4.5

4.0

inh()

]

10 K

0.15

0.10

0 05

1/B

(T-

0.8

x

x (T)

/

-6 0

-5.5

-5.0

n [

R/R

0Bsi

5 K

8 K

0.05

0.00543210

n

0.7

1086420T (K)

-6.5

-6.0

Ln

0.200.121/B (T-1)

1.9 K

Fig. 3n T (K) 1/B (T )

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0 8(a) (b) (c)300150

100

50(meV

)

This paper

0.8

0.7

0.6

(a.u

.)200150

meV

)

(a) (b) (c)300

250

Dirac0

-50

-100

E - E

D Analytis etc. [21]

Lang etc. [28] 0.5

0.4

0.3

dI/d

V

50

0

50

100

E-E

D(m Dirac

point

-10043210

ns (1012cm-2)-400 -300 -200 -100 0 100 200

E (meV)

-500.0-0.8 0.8

K//(Å-1)

Fig. 4

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