Abstract
Quantum Hall effect provides a simple way to study the competition between single particle physics and electronic interaction. However, electronic interaction becomes important only in very clean graphene samples and so far the trilayer graphene experiments are understood within noninteracting electron picture. Here, we report evidence of strong electronic interactions and quantum Hall ferromagnetism seen in Bernalstacked trilayer graphene. Due to high mobility ∼500,000 cm^{2 }V^{−1 }s^{−1} in our device compared to previous studies, we find all symmetry broken states and that Landaulevel gaps are enhanced by interactions; an aspect explained by our selfconsistent Hartree–Fock calculations. Moreover, we observe hysteresis as a function of filling factor and spikes in the longitudinal resistance which, together, signal the formation of quantum Hall ferromagnetic states at low magnetic field.
Introduction
Mesoscopic experiments tuning the relative importance of electronic interactions to observe complex ordered phases have a rich past^{1}. While one class of experiments were conducted on bilayer twodimensional electron systems (2DES) realized in semiconductor heterostructures, the other class of experiments focussed on probing multiple interacting subbands in quantum well structures^{2}. There is an increasing interest in the electronic properties of fewlayer graphene^{3,4,5,6,7,8,9,10,11,12,13} as it offers a platform to study electronic interactions because the dispersion of bands can be tuned with number and stacking of layers in combination with electric field. Bernal/ABAstacked trilayer graphene (ABATLG) provides a natural platform to observe such multisubband physics as the band structure gives rise to monolayerlike (ML) and bilayerlike (BL) bands. The presence of the multiple bands and their Dirac nature lead to the possibility of observing an interesting interplay of electronic interactions in different channels leading to novel phases of the quantum Hall state.
Here we study the Landaulevel (LL) spectrum on edge contacted ABATLG samples encapsulated in hexagonal boron nitride (hBN) flakes. We observe the coexistence of both massless and massive Dirac fermions in the form of parabolically dispersed LL crossing points at low magnetic field. At intermediate magnetic field we show that the LL fan diagram indicates that the electronelectron interactions lead to formation of symmetry broken spin and valleypolarized states. Our selfconsistent Hartree–Fock calculation supports the observed interaction enhanced LL gaps at the symmetry broken states. We also observe hysteretic transport showing the formation of quantum Hall ferromagnetic (QHF) states.
Results
Magnetotransport in ABAtrilayer graphene
Figure 1a shows the lattice structure of ABATLG with all the hopping parameters. We use Slonczewski–Weiss–McClure (SWMcC) parametrization of the tight binding model for ABATLG^{14,15} (with hopping parameters γ_{0}, γ_{1}, γ_{2}, γ_{5} and δ) to calculate its low energy band structure. Definitions of all the hopping parameters are evident from Fig. 1a, and δ is the onsite energy difference of two inequivalent carbon atoms on the same layer. Its band structure, shown in Fig. 1b consists of both ML linear and BL quadratic bands^{16,17}.
Figure 1c shows an optical image of the device where the ABATLG graphene is encapsulated between two hBN flakes^{18}. Fourprobe resistivity (ρ) of the device is shown in Fig. 1d. The low disorder in the device is reflected in high mobility ∼500,000 cm^{2 }V^{−1 }s^{−1} on electron side and ∼800,000 cm^{2 }V^{−1 }s^{−1} on hole side; this leads to carrier mean free path in excess of 7 μm (see Supplementary Fig. 1 and Supplementary Note 1 for mobility and mean free path calculation). We measured one single gated device and one dual gated device on which we studied the effect of electric field. We found that the electron side data is relatively insensitive for low electric field range (<0.01 Vnm^{−1}) (see Supplementary Fig. 2 and Supplementary Note 2 for dual gate device data). Due to the better quality of the single gated device we show the measurements done on the single gated device throughout the paper.
We next consider the magnetotransport in ABATLG that reveals the presence of LLs arising from both ML and BL bands. The LLs are characterized by the following quantum numbers: N_{M} (N_{B}) defines the LL index with M (B) indicating monolayer (bilayer)like LLs, +(−) denotes the valley index of the LLs and ↑ (←) denotes the spin quantum number of the electrons. All the data shown in this paper, are taken at 1.5 K. Figure 2a shows the measured longitudinal resistance (R_{xx}) as a function of gate voltage (V_{bg}) and magnetic field (B) in the low B regime (see Supplementary Fig. 3 and Supplementary Note 3 for more data at low magnetic field). Observation of LLs up to very high filling factor ν=118 confirms the high quality of the device. Along with the usual straight lines in the fan diagram, we find additional interesting parabolic lines which arise because of LL crossings. Figure 2b shows the calculated noninteracting density of states (DOS) in the same parameter range which matches very well with the measured resistance. We find that the low B data can be well understood in terms of noninteracting picture and it allows determination of the band parameters.
We now consider the LL fan diagram for a larger range of V_{bg} and B. Figure 3a shows the calculated^{14,15,16} energy dispersion of the spin degenerate LLs with B. All the band parameters of multilayer graphene are not known precisely, so, we refine relatively smaller band parameters γ_{2}, γ_{5} and δ a little over the known values for bulk graphite^{19} to understand our experimental data (see Supplementary Table 1 and Supplementary Note 3 for estimation of band parameters from experimental LL crossing points). We find γ_{0}=3.1 eV, γ_{1}=0.39 eV, γ_{2}=−0.028 eV, γ_{5}=0.01 eV and δ=0.021 eV best describe our data. Figure 3b shows the main fan diagram where the measured longitudinal conductance (G_{xx}) is plotted as a function of V_{bg} and B. Due to lack of inversion symmetry, valley degeneracy is not protected in ABATLG, it breaks up with increasing B and reveals all the symmetry broken filling factors as seen in Fig. 3b.
Figure 3c shows measured G_{xx} focusing on the ν=0 state, which shows a dip right at the charge neutrality point, evident for B>6 T. Corresponding Hall conductance (G_{xy}) shows a plateau at zero indicating the occurrence of the ν=0 state (see Supplementary Fig. 4 and Supplementary Note 4 for longitudinal and Hall resistance data showing ν=0 state). While, the ν=0 plateau has been observed in monolayer graphene^{20} and in bilayer graphene^{21} (for B more than ∼15–25 T), this is the first observation of ν=0 state in trilayer graphene at such low B. A marked reduction in disorder allows observation of the ν=0 state in our device.
Focusing on the electron side, Fig. 3d,e show the experimentally measured LL fan diagram and labelled LLs, respectively. We see that the presence of N_{M}=0 LL gives rise to a series of vertical crossings along the B axis as is expected from the LL energy diagram (Fig. 3a). The highest crossing along the B axis appears when N_{M}=0 crosses with N_{B}=2 LL at ∼5 T.
From the complex fan diagram, seen in Fig. 3d,e, we can see both above and below the topmost LL crossing (V_{bg}∼10 V and B∼5 T), N_{M}=0 LL is completely symmetry broken and N_{B}=2 LL quartet, on the other hand, becomes twofold split at ∼3.5 T. The crossing between N_{M}=0 and N_{B}=2 LLs gives rise to three ringlike structures. Calculated LL energy spectra near the topmost crossing (Fig. 3e, inset) shows that spin splitting is larger than valley splitting for N_{B}=2 LL but valley splitting dominates over spin splitting for N_{M}=0 LL. We note that valley splitting of N_{M}=0 is very large compared with other ML LLs; which arises because ML bands are gapped in ABATLG unlike in monolayer graphene. As one follows the N_{M}=0 LL down towards B=0 one observes successive LL crossings of N_{M}=0 with N_{M}=2, 3, 4..... The sharp abrupt bends in the fan diagram occur due to the change of the order of filling up of LLs after crossings and the fact that the horizontal axis is charge density (proportional to V_{bg} and not LL energy). When these crossings are extrapolated to B=0, we see that N_{M}=0 LL is valley split as expected from the LL energy diagram Fig. 3a.
Role of electronic interaction and theoretical simulation
We next discuss experimental signatures that point towards the importance of interaction. Observation of spin split N_{M}=0 LL at B∼2 T cannot be explained from the noninteracting Zeeman splitting for Γ∼1.5 meV on electron side, estimated from the Dingle plot. Also, the large ratio of transport scattering time to quantum scattering time indicates that small angle scattering is dominant, a signature of the longrange nature of the Coulomb potential^{22,23,24} (see Supplementary Fig. 5 and Supplementary Note 5 for Dingle plot analysis). We also measure activation gap for the symmetry broken states ν=2, 3, 4, 5, 7 at B=13.5 T, and find significantly higher gaps than the noninteracting spinsplitting. For ν=3 and 5, Fermi energy (E_{F}) lies in spinpolarized gap of N_{M}=0 LL in K_{−} and K_{+} valley respectively. Measured energy gap at ν=3 is ∼5.1 meV and at ν=5 is ∼2.8 meV, whereas free electron Zeeman splitting is ∼1.56 meV at B=13.5 T (see Supplementary Fig. 6, Supplementary Table 2 and Supplementary Note 6 for determination of LL energy gaps from Arrhenius plots). We note that typically the transport gap tends to underestimate the real gap due to the LL broadening, so actual single particle gap might be even larger. This shows the clear role of interactions even with a conservative estimate of the LL gap.
Interaction results in symmetry broken states at low B that are QHF states. For the data in Fig. 3d, ν=2, 3, 4, 5 are QHF states for B>5.5 T. Similarly, ν=7, 8, 9 are also QHF states for 5.5 T>B>4 T. In fact the LLs associated with ν=3, 4, 5 after crossing are the same ML LLs which are responsible for ν=7, 8, 9 before crossing (Fig. 3e). The crossings result in three ringlike structures marked by plus, triangle and hexagon in Fig. 3f.
Now we discuss theoretical calculations to show that electronic interactions are crucial in obtaining a quantitative understanding of the experimental data. The theoretical calculations focus on the N_{M}=0 and N_{B}=2 LLs, which form the most prominent LL crossing pattern in our data. The effect of disorder is incorporated within a selfconsistent Born approximation (SCBA)^{25,26}, while electronic interactions are included by considering the exchange corrections to the LL spectrum due to a statically screened Coulomb interaction^{27,28} in a selfconsistent way. Figure 4a shows the DOS at E_{F} as a function of V_{bg} and B, which matches with the experimental results on the G_{xx}.
Our calculations also provide insight about the polarization of the states inside the ringlike structures (Fig. 3f). We find that although the filling factor of region Δ is the same as that of regions ν=6 above and below, electronic configurations of these states are different. Figure 4b shows the spinresolved DOS at E_{F} as a function of V_{bg} and B. We find total spin polarization (integrated spin DOS) in region Δ is nonzero (see Supplementary Fig. 7 and Supplementary Note 7 for the details of theoretical calculation), but it vanishes in regions ν=6 above and below the ring structure. Figure 4b inset shows the calculated exchange enhanced spin gfactors. This shows a significant increase over bare value of g in the spinpolarized states—in agreement with the large gap observed at ν=3 and 5 in the experiment.
Discussion
The key role of interactions is also reflected in the hysteresis of R_{xx} in the vicinity of the symmetry broken QHF states. Though QHF has been extensively studied in 2DES using semiconductors^{2,29} there are only a few reports of studying QHF in graphene^{30,31,32,33}. In our experiment, we vary filling factor by changing V_{bg} at a fixed B (Fig. 5a) and observe that the sweep up and down of V_{bg} shows a hysteresis in R_{xx}, which can be attributed to the occurrence of pseudospin magnetic order at the symmetry broken filling factors^{34} (see Supplementary Fig. 8 and Supplementary Note 8 for more hysteresis data). Corresponding hysteresis is absent in simultaneously measured Hall resistance R_{xy} (Fig. 5b). Hysteresis in R_{xx} with V_{bg} is also absent without magnetic field (see Supplementary Fig. 8 and Supplementary Note 8 for more detail). The pinning, that causes the hysteresis could be due to residual disorder within the system as the domains of the QHF evolve. Along a constant filling factor ν=6 line (Fig. 5c) transport measurements show an appearance of R_{xx} spikes around the crossing of N_{M}=0 and N_{B}=2 LLs (Fig. 5d). One possible explanation for the spike in R_{xx} (ref. 35) is the edge state transport along domain wall boundaries as studied earlier in semiconductors^{29,36}.
In summary, we see interaction plays an important role to enhance the gfactor and favours the formation of QHF states at low B and at relatively higher temperature. ABATLG is the simplest system that has both massless and massive Dirac fermions, giving rise to an intricate and rich pattern of LLs that, through their crossings, can allow a detailed study of the effect of interaction at sufficiently low temperature. The ability to image these QHF states using modern scanning probe techniques at low magnetic fields could provide insight into these states that have never been imaged previously. In future, experiments on multilayer graphene, exchange coupled with a ferromagnetic insulating substrate^{37}, can lead to the possibility of observing an exciting interplay of QHF with the proximity induced ferromagnetic order.
Methods
Device fabrication
Graphene and hBN flakes were exfoliated by scotch tape method on 300 nm SiO_{2} coated highly pdoped Si substrate. hBN flakes of thickness ∼30 nm were located by an optical microscope. ABATLG was then transferred to a suitably chosen hBN, followed by another hBN transfer of similar thickness to complete the hBNgraphenehBN stack. Electronbeam lithography was done to define the contacts. Then the stack was etched with mild plasma in Argon and Oxygen (1:1 ratio) environment to expose the graphene edge. Metal (3 nm Chromium, 15 nm Palladium, 30 nm Gold) was thermally evaporated to make the contacts immediately after etching without breaking the vacuum.
Characterization
After exfoliation on Silicon substrate potential ABATLG graphene flakes were chosen by the optical colour contrast and then confirmed by the Raman spectroscopy. Atomic force microscopy was also done on the complete stack to image the topography of the surface and to find out the thickness of the top hBN which is required to calculate the plasma etching time before metallization.
Measurement
All the lowtemperature measurements were done in a liquid He_{4} flow cryostat at base temperature T=1.5 K. Standard low frequency lockin technique was used to do all current biased fourprobe resistance measurements. Excitation current was 100 nA for most of the measurements but sometimes increased to a higher value of 400 nA to measure low resistances at low magnetic fields.
Data availability
The data that support the findings of this study are available from the corresponding author upon request.
Additional information
How to cite this article: Datta, B. et al. Strong electronic interaction and multiple quantum Hall ferromagnetic phases in trilayer graphene. Nat. Commun. 8, 14518 doi: 10.1038/ncomms14518 (2017).
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References
 1.
Girvin, S. M. Spin and isospin: exotic order in quantum Hall ferromagnets. Phys. Today 53, 39–45 (2000).
 2.
Eom, J. et al. Quantum Hall ferromagnetism in a twodimensional electron system. Science 289, 2320–2323 (2000).
 3.
Yacoby, A. Graphene: Tri and tri again. Nat. Phys. 7, 925–926 (2011).
 4.
Taychatanapat, T., Watanabe, K., Taniguchi, T. & JarilloHerrero, P. Quantum Hall effect and Landaulevel crossing of Dirac fermions in trilayer graphene. Nat. Phys. 7, 621–625 (2011).
 5.
Bao, W. et al. Stackingdependent band gap and quantum transport in trilayer graphene. Nat. Phys. 7, 948–952 (2011).
 6.
Kumar, A. et al. Integer quantum Hall effect in trilayer graphene. Phys. Rev. Lett. 107, 126806 (2011).
 7.
Zhang, F., Tilahun, D. & MacDonald, A. H. Hund’s rules for the n=0 Landau levels of trilayer graphene. Phys. Rev. B 85, 165139 (2012).
 8.
Henriksen, E. A., Nandi, D. & Eisenstein, J. P. Quantum Hall effect and semimetallic behavior of dualgated ABAstacked trilayer graphene. Phys. Rev. X 2, 011004 (2012).
 9.
Craciun, M. F. et al. Trilayer graphene is a semimetal with a gatetunable band overlap. Nat. Nanotechnol. 4, 383–388 (2009).
 10.
Campos, L. C. et al. Landau level splittings, phase transitions, and nonuniform charge distribution in trilayer graphene. Phys. Rev. Lett. 117, 066601 (2016).
 11.
Lee, Y. et al. Broken symmetry quantum Hall states in dualgated ABA trilayer graphene. Nano Lett. 13, 1627–1631 (2013).
 12.
Stepanov, P. et al. Tunable symmetries of integer and fractional quantum Hall phases in heterostructures with multiple Dirac bands. Phys. Rev. Lett. 117, 076807 (2016).
 13.
Lee, Y. et al. Competition between spontaneous symmetry breaking and singleparticle gaps in trilayer graphene. Nat. Commun. 5, 5656 (2014).
 14.
McCann, E. & Fal’ko, V. I. Landaulevel degeneracy and quantum Hall effect in a graphite bilayer. Phys. Rev. Lett. 96, 086805 (2006).
 15.
Koshino, M. & McCann, E. Parity and valley degeneracy in multilayer graphene. Phys. Rev. B 81, 115315 (2010).
 16.
Serbyn, M. & Abanin, D. A. New Dirac points and multiple Landau level crossings in biased trilayer graphene. Phys. Rev. B 87, 115422 (2013).
 17.
Morimoto, T. & Koshino, M. Gateinduced Dirac cones in multilayer graphenes. Phys. Rev. B 87, 085424 (2013).
 18.
Wang, L. et al. Onedimensional electrical contact to a twodimensional material. Science 342, 614–617 (2013).
 19.
Dresselhaus, M. S. & Dresselhaus, G. Intercalation compounds of graphite. Adv. Phys. 51, 1–186 (2002).
 20.
Zhang, Y. et al. Landaulevel splitting in graphene in high magnetic fields. Phys. Rev. Lett. 96, 136806 (2006).
 21.
Zhao, Y., CaddenZimansky, P., Jiang, Z. & Kim, P. Symmetry breaking in the zeroenergy Landau level in bilayer graphene. Phys. Rev. Lett. 104, 066801 (2010).
 22.
Hwang, E. H. & Sarma, S. D. Singleparticle relaxation time versus transport scattering time in a twodimensional graphene layer. Phys. Rev. B 77, 195412 (2008).
 23.
Coleridge, P. T. Smallangle scattering in twodimensional electron gases. Phys. Rev. B 44, 3793 (1991).
 24.
Knap, W. et al. Spin and interaction effects in Shubnikovde Haas oscillations and the quantum Hall effect in GaN/AlGaN heterostructures. J. Phys. Condens. Matter 16, 3421 (2004).
 25.
Ando, T. Theory of quantum transport in a twodimensional electron system under magnetic fields ii. singlesite approximation under strong fields. J. Phys. Soc. Jpn 36, 1521–1529 (1974).
 26.
Zheng, Y. & Ando, T. Hall conductivity of a twodimensional graphite system. Phys. Rev. B 65, 245420 (2002).
 27.
Ando, T. & Uemura, Y. Theory of oscillatory g factor in an MOS inversion layer under strong magnetic fields. J. Phys. Soc. Jpn 37, 1044–1052 (1974).
 28.
Gorbar, E. V., Gusynin, V. P., Miransky, V. A. & Shovkovy, I. A. Broken symmetry ν=0 quantum Hall states in bilayer graphene: Landau level mixing and dynamical screening. Phys. Rev. B 85, 235460 (2012).
 29.
Poortere, E. P. D., Tutuc, E., Papadakis, S. J. & Shayegan, M. Resistance spikes at transitions between quantum Hall ferromagnets. Science 290, 1546–1549 (2000).
 30.
Nomura, K. & MacDonald, A. H. Quantum Hall ferromagnetism in graphene. Phys. Rev. Lett. 96, 256602 (2006).
 31.
Young, A. F. et al. Spin and valley quantum Hall ferromagnetism in graphene. Nat. Phys. 8, 550–556 (2012).
 32.
Lee, K. et al. Chemical potential and quantum Hall ferromagnetism in bilayer graphene. Science 345, 58–61 (2014).
 33.
Lee, Y. et al. Multicomponent quantum Hall ferromagnetism and Landau level crossing in rhombohedral trilayer graphene. Nano Lett. 16, 227–231 (2016).
 34.
Piazza, V. et al. Firstorder phase transitions in a quantum Hall ferromagnet. Nature 402, 638–641 (1999).
 35.
Muraki, K., Saku, T. & Hirayama, Y. Charge excitations in easyaxis and easyplane quantum Hall ferromagnets. Phys. Rev. Lett. 87, 196801 (2001).
 36.
Jungwirth, T. & MacDonald, A. H. Resistance spikes and domain wall loops in Ising quantum Hall ferromagnets. Phys. Rev. Lett. 87, 216801 (2001).
 37.
Wang, Z., Tang, C., Sachs, R., Barlas, Y. & Shi, J. Proximityinduced ferromagnetism in graphene revealed by the anomalous Hall effect. Phys. Rev. Lett. 114, 016603 (2015).
Acknowledgements
We thank Allan MacDonald, Jainendra Jain, Jim Eisenstein, Fengcheng Wu, Vibhor Singh, Shamashis Sengupta and Chandni U. for discussions and comments on the manuscript. We also thank John Mathew, Sameer Grover and Vishakha Gupta for experimental assistance. We acknowledge Swarnajayanthi Fellowship of Department of Science and Technology (for M.M.D.) and Department of Atomic Energy of Government of India for support. Preparation of hBN single crystals is supported by the Elemental Strategy Initiative conducted by the MEXT, Japan and a GrantinAid for Scientific Research on Innovative Areas ‘Science of Atomic Layers’ from JSPS.
Author information
Affiliations
Department of Condensed Matter Physics and Materials Science, Tata Institute of Fundamental Research, Homi Bhabha Road, Mumbai 400005, India
 Biswajit Datta
 , Hitesh Agarwal
 , Abhinandan Borah
 & Mandar M. Deshmukh
Department of Astronomy and Astrophysics, Tata Institute of Fundamental Research, Homi Bhabha Road, Mumbai 400005, India
 Santanu Dey
Department of Theoretical Physics, Tata Institute of Fundamental Research, Homi Bhabha Road, Mumbai 400005, India
 Abhisek Samanta
 & Rajdeep Sensarma
Advanced Materials Laboratory, National Institute for Materials Science, 11 Namiki, Tsukuba 3050044, Japan
 Kenji Watanabe
 & Takashi Taniguchi
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Contributions
B.D. fabricated the device, conceived the experiments and analysed the data. M.M.D., A.B. and B.D. contributed to the development of the device fabrication process. H.A. helped in the fabrication and in the measurements. K.W. and T.T. grew the hBN crystals. S.D., A.S. and B.D. did the calculations under the supervision of R.S.; B.D., M.M.D. cowrote the manuscript and R.S. provided input on the manuscript. All authors commented on the manuscript. M.M.D. supervised the project.
Competing interests
The authors declare no competing financial interests.
Corresponding authors
Correspondence to Rajdeep Sensarma or Mandar M. Deshmukh.
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