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Symmetry of superconducting correlations in displaced bilayers of graphene

Mohammad Alidoust,1 Morten Willatzen,2, 3 and Antti-Pekka Jauho4


1
Department of Physics, K.N. Toosi University of Technology, Tehran 15875-4416, Iran
2
Beijing Institute of Nanoenergy and Nanosystems, Chinese Academy of Sciences,
No. 30 Xueyuan Road, Haidian District, Beijing 100083, China
3
Department of Photonics Engineering, Technical University of Denmark, Kongens Lyngby, DK-2800, Denmark
4
Center for Nanostructured Graphene (CNG), DTU Nanotech,
Technical University of Denmark, DK-2800 Kongens Lyngby, Denmark
(Dated: April 26, 2019)
Using a Green’s function approach, we study phonon-mediated superconducting pairing symmetries that may
arXiv:1903.11623v2 [cond-mat.mtrl-sci] 24 Apr 2019

arise in bilayer graphene where the monolayers are displaced in-plane with respect to each other. We consider
a generic coupling potential between the displaced graphene monolayers, which is applicable to both shifted
and commensurate twisted graphene layers; study intralayer and interlayer phonon-mediated BCS pairings;
and investigate AA and AB(AC) stacking orders. Our findings demonstrate that at the charge neutrality point,
the dominant pairings in both AA and AB stackings with intralayer and interlayer electron-electron couplings
can have even-parity s-wave class and odd-parity p-wave class of symmetries with the possibility of invoking
equal-pseudospin and odd-frequency pair correlations. At a finite doping, however, the AB (and equivalently
AC) stacking can develop pseudospin-singlet and pseudospin-triplet d-wave symmetry, in addition to s-wave,
p-wave, f -wave, and their combinations, while the AA stacking order, similar to the undoped case, is unable to
host the d-wave symmetry. When we introduce a generic coupling potential, applicable to commensurate twisted
and shifted bilayers of graphene, d-wave symmetry can also appear at the charge neutrality point. Inspired by
a recent experiment where two phonon modes were observed in a twisted bilayer graphene, we also discuss the
possibility of the existence of two-gap superconductivity, where the intralayer and interlayer phonon-mediated
BCS picture is responsible for superconductivity. These analyses may provide a useful tool in determining the
superconducting pairing symmetries and mechanism in bilayer graphene systems.

I. INTRODUCTION our conclusions depend on having two different coupling


strengths (intralayer and interlayer couplings), and the mi-
croscopic details of the coupling do not matter. For exam-
Graphene, a two-dimensional honeycomb arrangement of
ple, the interlayer coupling could have a significant covalent
covalently bound carbon atoms, can be used as a basic build-
component.10–22 . In particular, recent experiments demon-
ing block for novel multilayer systems coupled by interlayer
strated the different intralayer and interlayer electron-phonon
van der Waals forces. These weak interlayer bonding forces
interactions by using a Raman spectroscopy technique: two
allow the possibility to create different ordering stacks that
resonance peaks in the Raman modes were observed by tun-
possess dramatically different low-energy properties, offering
ing the energy of excitation with IR and UV photons22 .
low-cost tools for rich band structure and material engineering
The electron-phonon coupling affects, for instance, the
perspectives. The ordering of the stacks can be controlled ex-
electronic mobility, thermal conductivity, and the (possi-
ternally by growth techniques or by the application of tensile
ble) superconducting phases. A recent landmark experiment
stress to laterally shift and/or rotate the layers in plane with
showed intrinsic superconductivity with a critical tempera-
respect to each other1–5 .
ture of ∼ 1.7 K in a twisted BLG, away from the charge
Depending on the stacking order, the multilayers can have neutrality point µ > 0 at a very low carrier density of
a number of different configurations. Bilayer graphene (BLG) 1011 cm−2 . Interestingly, the general features of the phase di-
where the top and bottom layers are mutually rotated is an ex- agram seemed to share the same phenomenology as high T c
ample of introducing additional features by a simple geomet- superconductors26 . Soon after, another experiment27 (and re-
ric action. It has been shown that at low angles of the twist, cently few others28–30 ) and a very large number of theoretical
the BLG develops a highly nontrivial band structure6–22 . An papers have appeared, many of which focus on the phonon-
efficient theory tool to approach such a problem and describe mediated single-gap superconductivity, and addressed various
its underlying physics is the effective Hamiltonian method. aspects of the observed superconducting phase (see, e.g. Refs.
This technique assumes that the two pristine graphene lay- [31–37, 42–49, 66–69]). However, earlier theories have not
ers are unaffected under the displacement and all changes can discussed the role of deformations in determining the super-
be translated into a new coupling potential between the two conducting properties of BLG50,52–54 .
layers23–25 . In this paper, we construct the Green’s function for various
Physically, one can expect that the charge carriers in coupling scenarios and present an extensive study of phonon-
BLG experience different interactions due to different phonon mediated pairing possibilities in BLG. As mentioned above,
modes generated within or between the layers. The two pris- a recent experiment has demonstrated two phonon modes in
tine graphenes have identical phonon modes (due to the in- a twisted BLG22 . One mode was attributed to the intralayer
tralayer covalent bonds) while a different mode appears due vibrations while the other mode was related to interlayer cou-
to the interlayer coupling (van der Waals bonds). Note that plings. Therefore, in the same spirit, one can expect that
2

BLG can potentially develop two-gap superconductivity in the We note that our analysis include the influence of chemical
phonon-mediated electron-electron coupling picture, where potential (away from the charge neutrality point) and are in-
each gap is mainly supported by one of the two phonon modes. dependent of the amplitude of the phonon-mediated electron-
Motivated by this picture, we also develop a two-gap super- electron interaction: ∆. We emphasize that our paper dis-
conductivity model for BLG. We employ the effective Hamil- cusses the possible symmetries of superconducting pair cor-
tonian method, consider a generic coupling matrix for the in- relations away from the magic angle of an incommensurately
terlayer coupling potential of BLG, and study the different twisted BLG.
superconducting pairings and correlations. The generic ex- In Sec. II, we first outline the Green’s function technique,
pressions we derive can be applied to both twisted and shifted the effective Hamiltonian approach, and discuss different pair-
BLG when using the appropriate coupling terms, as will be ing scenarios that may arise in BLG (some related discussions
discussed below. are presented in Appendix A). In Sec. III, we study the anoma-
For concreteness, we study shifted BLG with specific shift lous Green’s function both analytically and numerically for
directions so that AA stacking turns into AB, AB into AC, different scenarios in AA and AB stacking orders. We first
and AC into AA in the extreme limits of the shift. We find consider an undoped system and derive analytic expressions to
that for an undoped system, the anomalous Green’s func- the components of anomalous Green’s function in Sec. III A.
tion possesses only even-parity s-wave class and odd-parity Next, for a doped system, we evaluate the Green’s functions
p-wave class of symmetries for both AA and AB orderings numerically, and support these results by analytic expressions
with intralayer/interlayer phonon-mediated electron-electron given in Appendix B. In Sec. IV, we consider a generic cou-
coupling. For a doped system, however, AB ordering offers pling potential between the two pristine graphene layers and
a rich variety of pairing symmetries such as s-wave, p-wave, repeat our studies of Sec. II, now in the presence of a small
d-wave, f -wave, and symmetry combinations. On the other displacement between the two layers. We also study the tem-
hand, AA retains its previous even-parity s-wave, odd-parity perature dependencies of the superconducting gaps. We fi-
p-wave (now f -wave class) symmetries. Introducing a generic nally give concluding remarks in Sec. V.
coupling potential that accommodates in-plane twist and shift
between layers, a d-wave symmetry can appear for both AA
II. LOW ENERGY EFFECTIVE HAMILTONIAN AND
and AB orderings at µ = 0. Therefore, our findings suggest
GREEN’S FUNCTION APPROACH
that by shifting the layers of a BLG with respect to each other,
an effective switching to d-wave superconducting pairing with
specific pseudospin (Pspin) states is accessible. This phe- We follow the effective Hamiltonian strategy23–25 where the
nomenon offers a platform to control both superconducting Hamiltonian governing the low-energy physics of a generic
critical temperature and the Pspin degree of freedom of super- BLG involving an arbitrary in-plane displacement between the
conducting correlations by experimentally simple actions that layers can be expressed as
can find crucial applications in spintronics in addition to great
Z
dk †
interest to fundamental researches. The pairing symmetries H= ψ̂ (k)H(k)ψ̂(k) (1)
(2π)2
predicted here can be probed experimentally by point contact Z
dk † n o
tunneling spectroscopy experiments so that the conductance = 2
ψ̂ (k) H1 (k)ρ1 + H2 (k)ρ2 + T̃ (k)ρ+ + T̃ † (k)ρ− ψ̂(k),
in different directions will be different and reveals these sym- (2π)
metries. It is worth mentioning that similar theory study as the in which the layer degree of freedom is described in terms
present paper was conducted for black phosphorus monolayer of Pauli matrices ρ0,z,x,y , and we have defined 2ρ1 = ρ0 + ρz ,
in Ref. 51. It was found that a significant transition from ef- 2ρ2 = ρ0 − ρz , 2ρ+ = ρ x + iρy , 2ρ− = ρ x − iρy . The matrix
fective s-wave (p-wave) to d-wave ( f -wave) symmetry class T̃ (k) couples the top (1) and bottom (2) pristine single-layer
is accessible simply by the exertion of strain into the plane of graphene (SLG) and contains all information about the rela-
black phosphorus monolayer. tive displacement between the layers (see below)23–25 . The
Using the obtained anomalous Green’s function, we also Hamiltonians of the top and bottom layers are denoted by
calculate the intralayer and interlayer superconducting gaps H1,2 (k) = ~vF k · σ, respectively, in which σ = (σ x , σy ) and
as a function of temperature. For a given s-wave electron- σ x , σy are Pauli matrices. The multiplication of Pauli matri-
electron interaction potential, our results show that the in- ces ρi and σi implies a tensor product so that the Hamilto-
tralayer coupling in AA stacking order has both the largest nian (1) is a 4 × 4 matrix and the matrix T̃ (k) has an im-
gap amplitude and critical temperature, while the next largest plicit σ (refer to Eqs. (3) and (4) for further details). Here,
gap and critical temperature belongs to interlayer coupling in the two-dimensional momentum k is in the plane of SLG.
AB stacking order. Also, the shift between the layers has op- The field operator associated with the Hamiltonian is given by
posite effects on the gap and critical temperature of intralayer ψ̂† (k) = (ψ†1↑ , ψ†1↓ , ψ†2↑ , ψ†2↓ ) where the first index is 1 (2) for
and interlayer superconductivity in AA and AB orderings: the the top (bottom) SLG and the second index is ↑ (↓) for Pspin
displacement applied to AA stacking with intralayer coupling up -sublattice A- (Pspin down -sublattice B-). Note that, ac-
or AB stacking with interlayer coupling reduces both the gap cording to the mean-field definition of BCS superconductivity,
and critical temperature, while it enhances both of them for two electrons with opposite spins and momenta are coupled
AA stacking with interlayer coupling and for AB stacking through an attractive potential. This means that electron and
with intralayer coupling. hole excitations should be taken from opposite corners of the
3

ky
TABLE I. Sublattice positions of BLG for different stacking orders. (a)
b2 (c)
k1
Stacking→ AA AB AC
ν1,A = (0,0) (0,0) (0,0) G1
k0
ν1,B = 2(a1 + a2 )/3 2(a1 + a2 )/3 2(a1 + a2 )/3
A Γ kx
ν2,A = (0,0) (a1 + a2 )/3 2(a1 + a2 )/3
ν2,B = 2(a1 + a2 )/3 (0,0) (a1 + a2 )/3 B G2
k2 b1

Brillouin zone55–57 . In this case, one can show that the sys- (b) B
tem possesses spin degeneracy55–57 . Nonetheless, to denote A
the Pspin and keep our notation simplified simultaneously, we B
have dropped the spin and valley indices. A detailed discus- A
sion is presented in Appendix A.
We next define the parameters that characterize a BLG sys-
tem with a relative displacement between the top and bottom FIG. 1. (Color online). (a) Graphene monolayer in real space (cir-
SLG. The monolayer pristine graphene can be divided into cles stand for carbon atoms) that is described by primitive vectors
two sublattices A and B that can be described by two sublat- a1 and a2 . The plane of graphene is located in the xy plane and the
tice positions in real space νA = (0, 0), νB = 2(a √ 1 + a2 )/3 honeycomb lattice can be separated into two sublattices A and B. (b)
and two lattice vectors a1 = a(1, 0), a2 = a(1, 3)/2. Us- Illustration of an ideal AB stacking order where only the sublattice
ing this notation, the different stackings can be described by A of bottom layer (marked by red circles) is aligned with the sublat-
the sublattice positions given in Table I. Figure 1(a) displays tice B of top layer (marked by light blue circles). (c) Illustration of
K j = K0 + G j points in reciprocal space with primitive vectors b1
graphene lattice in real space with sublattices A and B marked
and b2 used in the calculations.
by dark red and dark blue circles, respectively. Also, we have
illustrated AB ordering in Fig. 1(b) where only the sublattice
B of top monolayer graphene is aligned with the sublattice
A of bottom layer. In AA case, A and B sublattices of the and MXX
j defines stacking order:
top layer are aligned with A and B sublattices of the bottom
e+i(2 jπ/3)
! !
layer (see Table I). The reciprocal lattice of a BLG √ can be 1 e−i(2 jπ/3) 1
j =
MAA , = ,
AB
M
described by√ the lattice vectors b1 = 2a−1 π(1, −1/ 3), b2 = e+i(2 jπ/3) 1 j e−i(2 jπ/3) e+i(2 jπ/3)
2a−1 π(0, 2/ 3) in reciprocal space as shown in Fig. 1(c). e−i(2 jπ/3) e+i(2 jπ/3)
!
Since we are interested in the low-energy physics, the Hamil- Mj =
AC
. (4)
1 e−i(2 jπ/3)
tonian can be expanded around reciprocal sublattice points:

K j = K0 + G j , (2) In what follows, we consider two types of couplings that


may lead to phonon-mediated superconductivity in a BLG22 .
in which K0 = (2b1 +b2 )/3, G0 = 0, G1 = −b1 , G2 = −b1 −b2 The top and bottom SLG are assumed to possess identi-
(see Fig. 1(b)). The periodic arrangement of atoms in SLG is cal phonon modes while the coupling between the two SLG
spanned by r = R j + να , where R j are integer combinations induces a new and different phonon mode22 . Thus, the
of the primitive lattice vectors a j , and the orbitals centered at BCS electron coupling within each layer is called ‘intralayer
positions να . In the following, r is the location at which the phonon-mediated electron-electron coupling’ and the electron
coupling between the top and bottom layers takes place. For coupling between the two layers is called ‘interlayer phonon-
example, the coupling of A and B sublattices shown in Fig. mediated electron-electron coupling’ throughout this paper. In
1(b). The displacement enters the coupling matrix T̃ via a this basis, the two types of pairing mechanisms are character-
phase factor23–25 , ized by the following two-electron amplitudes:

t⊥ (K j + k) i(K j +k)(u2 −u1 )


D E D E
X i) ∆S ψ†1↑ ψ†1↓ + h.c. and ∆S ψ†2↑ ψ†2↓ + H.c., (5a)
T̃ (k) = MXX
j e , (3)
3 D E
j=0,1,2 ii) ∆B ψ†1↑ ψ†2↓ + H.c. , (5b)

in which t⊥ (K j + k) is the interlayer hopping amplitude, givenE


P 1,i D † where ∆S and ∆B are the BCS spin-singlet phonon-mediated
by t⊥ (q) = Vu drt⊥ (r)e , t⊥ (r) = i, j t2, j r, 2 c2, j c1,i r0 , 1
R
−1 iqr
electron-electron coupling within each layer and between the
with c† , c being the creation and annihilation operators and layers, respectively. For more details see Appendix A.
r0 = r + δ in which δ denotes the distance between hopping We next consider the Green’s functions for the generic BLG
sites. Vu is the volume of unit cell, i, j run over the lattice system in the presence of superconductivity. The normal
sites, u1,2 are the displacements of the top and bottom layers, Green’s functions g and the anomalous Green’s function f are
4

defined as follows;51 local density of states. Hence, in what follows, we focus on


σσ0
the anomalous Green’s function fρρ and do not present ex-
gσσ
0 0
ρρ0 (τ, τ ; r, r ) = −hTτ ψρσ (τ, r )ψρ0 σ0 (τ , r )i,
0 0 0 † 0 0
(6a)
plicitly the normal Green’s function gσσ
0
ρρ0 although we have
gσσ0 (τ, τ0 ; r, r0 ) = −hTτ ψ†ρσ (τ, r)ψρ0 σ0 (τ0 , r0 )i,
0
(6b) derived all the components in our actual calculations.
ρρ
σσ0 In the following, inspired by the atomic orbital symbols,
0 (τ, τ ; r, r ) = +hTτ ψρσ (τ, r)ψρ0 σ0 (τ , r )i,
0 0 0 0
fρρ (6c)
we use the following nomenclature: terms proportional to
σσ0 †
fρρ0 (τ, τ0 ; r, r0 ) = +hTτ ψ†ρσ (τ, r)ψ†ρ0 σ0 (τ0 , r0 )i, (6d) k± (=k x ± iky ) → p-wave, k±2 → d-wave, and k±2 k∓ → f -wave,
etc. (see also Tables II and III).
where Tτ is the time ordering operator, and τ, τ0 are the imag-
inary times. Here, σ, σ0 and ρ, ρ0 denote the Pspin and layer In Secs. III A and III B, we consider undoped µ = 0 and
indices and h...i is the thermodynamics averaging. In particle- doped µ , 0 BLG, respectively. Each of these sections stud-
hole space, the Green’s function satisfies: ies both AA and AB orderings with both intralayer ∆S and
interlayer ∆B phonon-mediated electron-electron interaction.
∆(r)
ˆ
!
Ĥ(r) − iωn
ǧ(iωn ; r, r0 ) = δ(r − r0 ),(7)
∆ˆ ∗ (r) Tt Ĥ(r)Tt† + iωn
in which ωn = π(2n+1)kB T is the Matsubara frequency, n ∈ Z,
kB is the Boltzman constant, T is temperature, Tt is the time- A. Undoped bilayer graphene: µ = 0
reversal operator, and ∆(r)ˆ is the superconducting gap. Note
that Ĥ(r) is obtained by replacing k → −i∇ in H(k), in Eq. We consider two cases separately: spin singlet intralayer
(1). The matrix form of the Green’s function is given by; phonon-mediated electron-electron coupling ∆S and spin-
singlet interlayer phonon-mediated electron-electron coupling
ĝ(iωn ; r, r0 ) fˆ(iωn ; r, r0 )
!
ǧ(iωn ; r, r0 ) = ˆ† . (8) ∆B . In both cases, we assume a constant coupling potential be-
f (iωn ; r, r0 ) ĝ(iωn ; r, r0 ) tween the two monolayers given by: t = t† . The components
of coupling potential are defined by Eq. (3).
We denote 4×4 matrices by ‘hat’ symbol, , ˆ and 8×8 matrices
by ‘check’ symbol, . ˇ
We now proceed to derive the anomalous Green’s function
f for the different coupling scenarios (Eq. (17) below gives
the self-consistency condition these functions must satisfy).51 1. Intralayer coupling: ∆S , 0, ∆B = 0

•AA stacking: In this case, the components of the anoma-


III. BILAYER GRAPHENE WITHOUT ANY lous Green’s function Eqs. (6) are:
DEFORMATIONS

To begin, we consider spin-singlet intralayer and interlayer Ω f11


↑↑
= 0, (9a)
phonon-mediated electron-electron couplings and find pos- Ω f11
↑↓
= −∆S (k− k+ + t2 + ∆2S + ω2n ), (9b)
sible superconducting pair correlations in a BLG with zero
doping. We thus assume that the top and bottom SLG host Ω f12
↑↑
= −2t∆S k− , (9c)
identical phonon-mediated electron-electron interactions, i.e., Ω f12
↑↓
= 0, (9d)
∆1S ≡ ∆2S . In what follows, we use a compact notation for the
different combinations of momenta (see Table II) that arise Ω f11
↓↑
= +∆S (k− k+ + t + 2
∆2S + ω2n ), (9e)
during the calculations to simplify the resulting expressions. Ω f11
↓↓
= 0, (9f)
We first consider the simplest cases that result in analytic solu-
tions and gradually add parameters to reach more complicated Ω f12
↓↑
= 0, (9g)
low-energy effective Hamiltonians. Ω f12
↓↓
= +2t∆S k+ (9h)
This section is split into two subsections, where we study
Ω= k−2 k+2 + 2k− k+ (∆2S −t +
2
ω2n ) + (t +
2
∆2S + ω2n )2 . (9i)
the undoped and doped cases, respectively, considering both
AA and AB stacking orders. For symmetry reasons, the AC
stacking order leads to similar results as AB stacking and, As seen, the intralayer Pspin-triplet and interlayer Pspin-
thus, we omit presenting results for the AC stacking order. singlet correlations are not induced while, as expected, the
We also assume that the system is translationally invariant in intralayer Pspin-singlet pairings are nonzero and have even-
the xy plane (the plane of BLG) and thus the corresponding parity even-frequency symmetry. Interestingly, the Pspin-
Hamiltonian is diagonal in momentum space as a function triplet interlayer correlations are nonzero, proportional to the
of k x and ky . Consequently, we deal with a set of algebraic coupling strength between the layer and possess odd-parity
equations in momentum space for the Green’s function. The even-frequency symmetry.
σσ0
anomalous components of Green’s function fρρ 0 correspond •AB stacking: Next, we consider AB stacking order and in-
to pairing correlations that may arise in the system whereas tralayer opposite-spin phonon-mediated electron-electron in-
the normal Green’s function gσσ
0
ρρ0 contains information about teractions. Constructing the anomalous Green’s function, we
5

TABLE II. Different combinations of momentum functions, appearing in the calculations.

k+ = k x + iky k+2 = k2x + 2ik x ky − ky2 k+3 = k3x + 3ik2x ky − 3k x ky2 − iky3 k+4 = k4x + 4ik3x ky − 6k2x ky2 − 4ik x ky3 + ky4
k− = k x − iky k− = k x − 2ik x ky − ky
2 2 2
k−3 = k3x − 3ik2x ky − 3k x ky2 + iky3 k−4 = k4x − 4ik3x ky − 6k2x ky2 + 4ik x ky3 + ky4
k+ k− = k x + ky
2 2
k+ k− = (k x + ky )
2 2 2 2 2
k+3 k−3 = (k2x + ky2 )3 k+4 k−4 = (k2x + ky2 )4
k− k+ = k x − ik x ky + k x ky − iky
2 3 2 2 3
k− k+ = k x + ik x ky + 2k x ky + 2ik2x ky3 + k x ky4 + iky5
2 3 5 4 3 2

k− k+ = k x − 2ik x ky − 2ik x ky − ky
3 4 3 3 4
k+ + k− = 2k x
k−3 k+2 = k5x − ik4x ky + 2k3x ky2 − 2ik2x ky3 + k x ky4 − iky5 k+ − k− = 2iky

find: •AA stacking:

Ω f11
↑↑
= 0, (11a)
Ω f11
↑↓
= −2it∆B ωn , (11b)
Ω f11
↑↑
= 0, (10a) Ω f12
↑↑
= 0, (11c)
Ω f11
↑↓
= −∆S (k− k+ + ∆2S + ω2n ), (10b) Ω f12
↑↓
= −∆B (k− k+ − t + 2
∆2B + ω2n ), (11d)
Ω f12
↑↑
= −it∆S ωn , (10c) Ω f11
↓↑
= 2it∆B ωn , (11e)
Ω f12
↑↓
= 0, (10d) Ω f11
↓↓
= 0, (11f)
Ω f11
↓↑
= +∆S (k− k+ + ∆2S + ω2n ), (10e) Ω f12
↓↑
= ∆B (k− k+ − t + 2
∆2B + ω2n ), (11g)
Ω f11
↓↓
= 0, (10f) Ω f12
↓↓
= 0, (11h)
Ω f12
↓↑
= t∆S (k− − k+ ), (10g) Ω = (k− k+ − t + 2
∆2B )2 + 2(k− k+ + t + 2
∆2B )ω2n + ω4n .(11i)
Ω f12
↓↓
= +it∆S ωn , (10h)
Ω = (k− k+ + ∆2S )2 + (2k− k+ + t + 2
2∆2S )ω2n + ω4n . (10i) •AB stacking:

Ω f11
↑↑
= 0, (12a)
Ω f11
↑↓
= −t∆B k+ , (12b)
Similar to the AA case, the intralayer Pspin-triplet correla- Ω f12
↑↑
= 0, (12c)
tions are zero while the Pspin-singlet pairings are nonzero
with even-parity even-frequency. Due to the specific coupling Ω f12
↑↓
= −∆B (k− k+ + ∆2B + ω2n ), (12d)
matrix in the AB stacking order, one of the Pspin-singlet cor- Ω f11
↓↑
= t∆B k+ , (12e)
relation components is odd-parity and even in frequency while
the Pspin-triplet ones are even in parity and odd in frequency. Ω f11
↓↓
= 0, (12f)
Note that these unconventional correlations are proportional Ω f12
↓↑
= ∆B (k− k+ + t2 + ∆2B + ω2n ), (12g)
to the interlayer coupling strength t.
Ω f12
↓↓
= 0, (12h)
Ω= k−2 k+2 + 2k− k+ (∆2B + ω2n ) + (∆2B + ω2n )(∆2B + t + ω2n(12i)
2
).

Comparing with the Green’s function components of the


same stacking orders but with intralayer phonon-mediated
electron-electron coupling discussed in Subsec. III A 1, we
readily find that the AA stacking in the current scenario de-
velops even-parity and odd-frequency superconducting cor-
2. Interlayer BCS coupling: ∆S = 0, ∆B , 0 relations similar to the AB stacking order of Sec. III A 1.
The same symmetry correspondence can be seen between AB
stacking of this current subsection and Sec. III A 1. In that
Here, we consider a situation where one electron from the case, BLG develops odd-parity even-frequency correlations.
top layer and one from the bottom layer are coupled through Note that, unlike the intralayer phonon-mediated electron-
the interlayer phonons which is given by Eq. (5b). For AA and electron coupling scenario, Sec. III A 1, here all components
AB stack orderings of the two monolayer graphene, we find of the anomalous Green’s function are spin-singlet. Also, the
the following anomalous components of the Green’s function, odd-parity components are of p-wave type (i.e., proportional
Eqs. (6); to k± . See Tables II and III). Thus, for the undoped case, the
6

only possible pairing correlations with the intralayer and in- 2. AB stacking order: phonon-mediated intralayer and interlayer
terlayer phonon-mediated electron-electron couplings are of electron-electron couplings
s-wave and p-wave class regardless of the stacking order.
Figure 3 shows the pairing correlations in a BLG with AB
ordering of the top and bottom pristine layers. In Fig. 3(a), the
B. Bilayer graphene with finite doping µ , 0 BCS electron-electron coupling is of the intralayer type, i.e.,
∆S , 0, ∆B = 0, while Fig. 3(b) contains results with inter-
layer BCS electron-electron coupling, i.e., ∆S = 0, ∆B , 0.
Next, we consider finite doping, and reinvestigate the su- Clearly, in Fig. 3(a), components f11 , f12 , f11 , f12 show a
↑↓ ↑↑ ↓↑ ↓↓
perconducting correlations given by the anomalous Green’s combination of d-wave and s-wave symmetries both in imag-
function as discussed in the previous section. inary and real parts. The rest of the pairing components are,
however, of the p-wave and f -wave type similar to the AA or-
dering case we considered before. These observed odd-parity
1. AA stacking order: phonon-mediated intralayer and interlayer and d-wave (proportional to single k±2 ) symmetries can be con-
electron-electron couplings firmed by the analytic expressions in Eqs. (B2). In Fig. 3(b),
for the interlayer BCS coupling, the only component that pos-
↓↓
In the presence of a finite doping, analytic expressions for sesses effective d-wave symmetry is f11 . Checking through
↓↓
the anomalous Green’s function become cumbersome. How- Eqs. (B4), we see that f11 expression contains single k+2 which
ever, they allow one to deduce and analyze the pairing sym- produces the d-wave symmetry. The components f11 , f12 , f12
↑↑ ↑↓ ↓↑

metries that may arise. We have presented them in Appendix are of effective s-wave type while f11 , f12 , f11 , f12 show p-
↑↓ ↑↑ ↓↑ ↓↓
B and exploit them as a benchmark for our numerical calcula- wave symmetry beside terms proportional to k+ k−2 k+2 and k+2 k− .
tions. ↓↓
Mathematically, the reason that f11 gains d-wave symmetry is
To evaluate the effective momentum dependencies, we set
the specific combination of the interlayer coupling T̃ which
the Matsubara frequency fixed at the lowest mode with n = 0
has off-diagonal terms, and the phonon-mediated electron-
for the individual components of the anomalous Green’s func-
electron coupling ∆B that is on the off-diagonal entries of Eq.
tion evaluated at low temperatures (typically, T ∼ 0.01T c ).
(7).
We also set a ‘representative’ ratio to the chemical poten-
Our prediction of the symmetry changes and generation of
tial over coupling strength µ/t = 1.5 throughout the numer-
Pspin superconducting correlations can be confirmed exper-
ical study without loss of generality. Figure 2 illustrates the
imentally. A relevant experiment that can reveal distinctive
momentum space map of the real and imaginary parts of the
and direct evidence for the prediction of symmetry change is a
Green’s function components in AA stacking order. In Fig.
high-resolution angular point-contact tunneling spectroscopy
2(a), the phonon-mediated electron-electron coupling is of the
experiment. The angular tunneling spectroscopy experiment
intralayer type ∆S , 0, ∆B = 0 while in Fig. 2(b) we consider
can determine the angular dependence of superconducting
only interlayer coupling ∆S = 0, ∆B , 0. For the intralayer
correlations before and after introducing the displacement and
coupling, Pspin-singlet f11 , f12 , f11 , f12 components are real
↑↓ ↑↓ ↓↑ ↓↑
twist into the layers. Therefore, one should be able to distin-
and have s-wave (∝ k x + ky ) symmetry while the other compo-
2 2
guish between angle-independent and angle-dependent sym-
nents with triplet Pspin state show p-wave (∝ k± ) and f -wave metry classes. Another method that might be utilized in inves-
(∝ k±2 k∓ ) symmetries with both nonzero imaginary and real tigating the change in the symmetry profile of superconduct-
parts. The interlayer coupling changes this picture slightly. ing correlations discussed above is nonlinear Meissner effect
Yet, the correlations with triplet Pspin state are of effective f - to image the symmetry profile of pairing correlations58 .
wave class while the intralayer Pspin-singlet correlations are
purely imaginary with s-wave (∝ k2x + ky2 ) symmetry class.
↑↓ ↓↑
The interlayer Pspin-singlet correlations, f12 and f12 , are of
IV. SHIFTED AND TWISTED BILAYER GRAPHENE
s-wave class and even in frequency.
In short, the AA stacking order with and without dop-
ing and in the presence of intralayer or interlayer phonon- To study twisted BLG, one can assume that the top and
mediated electron-electron BCS coupling does not support d- bottom layers are rotated mutually by an amount of θ/2, one
wave symmetry class. Hence, AA stacking order can only clockwise and the other counter clockwise. Therefore, the un-
yields s-wave, p-wave, and f -wave type superconducting cor- coupled single layers can be described by H1,2 S
(±θ/2, θk ) =
relations with the phonon-mediated scenarios considered in Θz (±θ/2)H (θk )Θz (±θ/2), where θk is the direction of the par-
S †

this paper. This can be fully confirmed by examining the ana- ticles’ momentum in each layer and Θz (θ) is the rotation op-
lytic expressions given by Eqs. (B1) and (B3) in Appendix B. erator around the z axis perpendicular to the graphene plane.
According to the momentum combinations presented in Table In this case, the twist affects the coupling matrix as well so
II, Eqs. (B1) and (B3) contain no term of type single k±2 that that one finds T̃ (θ, r, k) from Eq. (3), now with the phase
results in d-wave symmetry class. The allowed momentum factor exp(ig · r) in which g j = Θz (+θ/2)G j − Θz (−θ/2)G j .
combinations are either odd-parity or possess s-wave symme- For commensurate rotation angles, e.g., θ = 21.787◦ , 38.213◦
try. one finds an effective 4 × 4 Hamiltonian in the momentum
7

FIG. 2. (Color online). Real and imaginary parts of the different pairing amplitudes in a BLG with perfect AA stacking and finite doping
µ , 0. (a) Pure intralayer coupling: ∆S , 0 and ∆B = 0. (b) Pure interlayer coupling: ∆S = 0 and ∆B , 0.

FIG. 3. (Color online). Real and imaginary parts of different pairings amplitudes in a BLG with a perfect AB stacking at finite doping µ , 0.
(a) Pure intralayer coupling: ∆S , 0 and ∆B = 0. (b) Pure interlayer coupling: ∆S = 0 and ∆B , 0.

space for the twisted BLG6,7 . As the twisting angle becomes with four different components for the coupling term, namely:
smaller, the superlattice cell gets larger. Note that for the non- !
commensurate angles, the bilayer system is inhomogeneous t11 t12
in real space and a very large basis set is needed to describe T̃ = , (13)
t21 t22
it59–69 . Also, an AA-stacked bilayer can be transformed into
an AB stacking order by keeping layer 1 fixed, i.e. u1 = 0, and and derive the anomalous Green’s function, and finally, inves-
shifting layer 2 by u2 = (a1 + a2 )/3 in Eq. (3). One can eas- tigate a specific case of shifted BLG. Note that our analytic
ily show that this transformation changes AA order into AB, results below are applicable to twisted BLG where the low-
AB into AC, AC into AA when  is equal to unity. energy physics can be described by the effective Hamiltonian
approach. One simply needs to replace appropriate coupling
Nevertheless, in what follows, we consider a generic matrix terms (i.e., t11 , t12 , t21 , t22 ), describing a twist.
8

FIG. 4. (Color online). Real and imaginary parts of different pairings for a nonideal AA stacking configuration, i.e., in which the top SLG
is shifted toward the AB configuration,  = 0.2, at finite doping, µ , 0 similar to the ideal AA stacking counterpart. (a) Purely intralayer
coupling: ∆S , 0 and ∆B = 0. (b) Pure interlayer coupling: ∆S = 0 and ∆B , 0.

FIG. 5. (Color online). Real and imaginary parts of different pairings for a nonideal AB stacking configuration, i.e., in which the top SLG is
shifted toward AC stacking,  = 0.2, at finite doping, µ , 0 similar to the ideal AB stacking counterpart. (a) Pure intralayer coupling: ∆S , 0
and ∆B = 0. (b) Pure interlayer coupling: ∆S = 0 and ∆B , 0.

As an illustrative example, we consider the pristine case, ∆B = 0. The results for the anomalous Green’s function are:
µ = 0, and only include the intralayer coupling: ∆S , 0, Ω f11
↑↑
= 0, (14a)
 
Ω f11
↑↓
= −∆S ∆2S + k− k+ + t11 t22 − t12 t21 + ω2n , (14b)
Ω f12
↑↑
= −∆S k− (t22 + t22

) − i∆S ωn (t12 + t21

), (14c)
Ω f12
↑↓
= −∆S (−k− t21 + ∗
k+ t21 − iωn (t11 − t22∗
)), (14d)
 
Ω f11
↓↑
= +∆S ∆2S + k− k+ + t11 t22 − t12 t21 + ω2n , (14e)
Ω f11
↓↓
= 0, (14f)
Ω f12
↓↑
= ∗
−∆S (−k− t12 + k+ t12 − iωn (t11∗
− t22 )), (14g)
Ω f12
↓↓
= +∆S k+ (t11 + t11 ) + i∆S ωn (t12 + t21 ),
∗ ∗
(14h)
9
     
Ω = k−2 k+2 − t12 ∗
t21 + k− −k+ −2 ∆2S + ω2n + and, subsequently, at large values of  recovers either AA,

t11 t22 + t11
∗  ∗
t22 − iωn (t12 (t11 + t22 ) + t21 (t11

+ t22

))
 AB, or AC symmetries depending on the initial ordering we
start with. In the next section, we see how this deformation

−k+2 t12 t21 − ik+ ωn (t21

(t11 + t22 ) + t12 (t11

+ t∗ )) + affects the critical temperature and superconducting gap and
  22
ω2n 2∆2S + t11 t11

+ t12 t12

+ t21 t21

+ t22 t22

− link them to the superconducting correlations discussed so far.
   As mentioned in passing, inspired by recent experiments
−∆2S − t11 t22 + t12 t21 ∆2S + t11 ∗ ∗ ∗ ∗
t22 − t12 t21 + ω4n . (15) in normal state26,27 , BLG may develop a “two-gap” super-
conductivity if the electron-electron coupling strength within
An examination of these equations leads to the following con-
the layers is unequal to the electron-electron coupling be-
clusions. Similar to Sec. III A, the generic coupling matrix
tween the two layers. Following this idea, we have calcu-
leads to vanishing f11 , f11 . However, the symmetries are no
↑↑ ↓↓
lated the anomalous Green’s function when both ∆S and ∆B
longer similar to those explored in Sec. III A. As seen, here, are nonzero. The results of this two-gap superconductivity
Ω includes terms of single k±2 that makes substantial changes. scenario are given by Eqs. (B5) of the Appendix. In deriv-
These terms have d-wave symmetry and thus the resultant ing Eqs. (B5) we consider bulk properties , i.e., ∆ = ∆† and
Green’s functions and corresponding superconducting corre- assume that the two layers develop identical superconducting
lations can now carry this symmetry as well. gap ∆S , which is unequal to the interlayer superconducting
Next, we consider the interlayer coupling (∆S = 0, ∆B , 0 gap ∆B . To be specific, we consider twisted bilayers by an
at µ = 0). The pairing correlations are given in Eqs. (16): amount θ with zero doping, i.e., µ = 0. The intralayer Pspin-
Ω f11
↑↑
= 0, (16a) triplet components remains zero. Similarly to the single gap
superconductivity case, Ω contains k±2 terms due to nonzero
Ω f11
↑↓
= ∆B (k− t21 + k+ t12 + iωn (t11 + t22 )), (16b) coupling potential terms considered.
Ω f12
↑↑
= ∗
i∆B (t21 ∗
t22 − t12 t22 ), (16c)
 
Ω f12
↑↓
= −∆B ∆B + k− k+ − t11 t22
2 ∗
+ ∗
t21 t21 + ω2n , (16d) A. Temperature dependence of superconducting gaps
Ω f11
↓↑
= ∆B (k− t21 + k+ t12 + iωn (t11 + t22 )), (16e)
Recalling Eqs. (B1)-(B4), the AB-stacked graphene bilayer
Ω f11
↓↓
= 0, (16f) with finite doping can potentially support a number of dif-
 
Ω f12
↓↑
= ∆B ∆2B + k− k+ − t11

t22 + t12 t12

+ ω2n , (16g) ferent pairings: s-wave, p-wave, d-wave, f -wave, and their
combinations. In addition to the anomalous Green’s function,
Ω f12
↓↓
= −i∆B (t11 t12
∗ ∗
− t11 t21 ), (16h) an interaction potential V(k, k0 ) enters the equations, deter-
Ω = −∆4B − k−2 k+2 + k−2 t12 ∗
t21 − 2∆2B k− k+ − mining the superconducting gap function and critical temper-
  ature. In general, the superconducting gap function can be
ω2n 2∆2B + 2k− k+ + t11 t11 ∗
+ t12 t12

+ t21 t21

+ t22 t22

+
momentum dependent and it satisfies the following equation
iωn (k− t12 (t11 + t22 ) + k− t21 (t11 + t22 ) + k+ t21 (t11 + t22 ) +
∗ ∗ ∗ ∗
that should be solved self-consistently together with Eq. (7):

k+ t12 (t11 + t22

)) + k− k+ t11 t22

+ k− k+ t11

t22 + k+2 t12 t21

− X
αα0 ,σσ0
∆αα 0 σσ0 0
0
ββ0 (k) = − Vββ0 ,ρρ0 (k, k ) fρρ0 (k ), (17)
t11 t11 t22 t22 + t11 t12 t21 t22 + ∆B t11 t22 + t11 t12 t21 t22 + ∆2B t11
∗ ∗ ∗ ∗ 2 ∗ ∗ ∗ ∗
t22
k0
−∆B t12 t12 − t12 t12 t21 t21 − ∆B t21 t21 − ωn .
2 ∗ ∗ ∗ 2 ∗ 4
in which α, α0 , β, β0 are Pspin and layer indexes, respectively.
We see that here, also , f11
↑↑ ↓↓
are zero. Similarly to the
f11 The interaction potential can be both spin and layer depen-
previous case, Ω includes single k±2 terms, carrying d-wave dent. Therefore, one can expand the interaction potential in
symmetry. Note that these single k±2 terms are not vanishing spherical harmonics and in terms of the atomic orbital sym-
here because all the entries of coupling matrix T̃ are assumed bols introduced in Table III.
nonzero with no specific symmetry. In all the previous cases, The type and details of phonon-mediated electron-electron
with specific stacking orders, Ω includes powers of k± k∓ that interactions can be obtained through optical absorption and
carry s-wave symmetry.
At finite doping, the expressions become cumbersome, and
we resort to numerical investigations. To examine the effect of TABLE III. Phonon mediated electron-electron interaction poten-
displacement on the effective symmetry profile of pairing cor- tials.
relations, we study the shifted BLG scenario numerically. Fig-
ures 4 and 5 are shifted ( = 0.2) counterparts of Figs. 2 and 3. Vs ∝ 1 Vextended−s ∝ k2x + ky2
When comparing these figures, we see that, for AA stacking, V px ∝ k x
the shift has induced imaginary parts into f11 , f11 , f12 , f12
↑↓ ↓↑ ↑↓ ↓↑
Vdxy ∝ k x ky Vdx2 −y2 ∝ k2x − ky2
pairings with intralayer coupling and real parts for the inter-
V fy(3x2 −y2 ) ∝ ky (3k2x − ky2 )
layer coupling. Also, in the case of AB stacking, this displace-
ment gives rise to nonzero real parts into f12 , f12 with ∆S , 0
↑↓ ↓↑ Vgxy(x2 −y2 ) ∝ Vgx4 +y4 ∝ k2x (k2x − 3ky2 )
k x ky (k2x − ky2 ) −ky2 (3k2x − ky2 )
and nonzero imaginary parts into f11 , f12 with ∆B , 0. In all
↑↑ ↑↓

cases, the displacement tends to first destroy the symmetries


10

1 1 1 1
(a) (b) (c) (d)
0.8 0.8 0.8 0.8

0.6 0.6 0.6 0.6

0.4 0.4 0.4 0.4

0.2 0.2 0.2 0.2

0 0 0 0
0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1 0 0.2 0.4 0.6 0.8 1

FIG. 6. (Color online). Temperature dependence of intralayer ∆S and interlayer ∆B superconducting gaps for different stacking orders. The
gap functions and temperature are normalized with respect to the intralayer gap at zero temperature for AA stacking without displacement,
i.e., ∆AA
S (T = 0) and its critical temperature, i.e., T c,S , respectively.
AA

Raman spectroscopy experiments10–22 . With the relevant intralayer and interlayer BCS coupling, respectively, induces
↑↓ ↑↓
anomalous Green’s functions at hand, Eqs. (B1)-(B5), it is nonzero imaginary parts to f11 and f12 that changes slightly
sufficient to insert the interaction potential into Eq. (17) to ob- the gap function and critical temperature, Figs. 6(a) and 6(d).
tain a self-consistent equation for the gap function, and solve One can repeat the study presented in Fig. 6 for other in-
it at different temperatures. As an example, we consider s- teraction types given in Table III and the given Green’s func-
wave pairing (i.e., V s in Table III) and plot the superconduct- tions in Eqs. (B1)-(B5). Nevertheless, we postpone such a
ing gap as a function of temperature for different scenarios study to future works when more details of interactions or rel-
presented in Fig. 6. Note that we have used an identical in- evant experimental data are available. It is, however, appar-
teraction potential for intralayer and interlayer coupling po- ent that considering d-wave or g-wave interactions in Table
tential in AA and AB orderings and set µ/t = 1.5 through- III for the electron-electron coupling potential V(k, k0 ) with
out our calculations (increasing the density of charged par- its spin state being singlet, the ratio of superconducting gap
ticles enhances the superconducting gap and critical temper- and critical temperature increases (according to the traditional
ature). With these assumptions, we find that the intralayer calculations of such interaction potentials70 ) for cases where
phonon-mediated electron-electron coupling in AA ordering the Green’s function itself possesses d-wave symmetry, as dis-
hosts the largest superconducting gap that, from energy point cussed in the previous section. Therefore, such a discussion
of view, results in the lowest ground-state energy. We thus should be relevant for the recent experiment26 that observed
normalize all other superconducting gaps and temperature by a puzzling behavior combining the features of high T c and
the intralayer zero temperature superconducting gap of AA conventional superconductors. Accordingly, by deforming the
ordering, i.e., ∆AAS (T = 0) and its critical temperature T c,S ,
AA
BLG, d-wave spin-singlet pairing may become dominant and
respectively. Figure 6 illustrates that the interlayer phonon- increase the ratio of the superconducting gap and T c .
mediated electron-electron coupling in AA ordering results in In our calculations above, we have simply followed the
the smallest critical temperature (Fig. 6(a)) while its AB or- BCS picture of superconductivity where the coupling of two
dering counterpart Fig. 6(d) has the closest gap amplitude and particles with opposite spins and momenta are building blocks
critical temperature to the intralayer AA ordering (the largest of superconductivity. Additionally, we have assumed that
one). We have also applied a small displacement, i.e.,  = 0.2, the influence of twist and displacement in superconducting
according to the discussion in the previous subsection. Com- BLG are encoded in the coupling terms of Eq. (13) and the
pairing Figs. 6(a) and 6(d), we find that the intralayer and electron-electron coupling interaction potentials remain un-
interlayer couplings in AA and AB stacking orders share sim- changed. Nevertheless, if twist and displacement change the
ilar behavior in all features in the presence and absence of amplitude of electron-electron coupling interaction potentials
the displacement. While the displacement in intralayer cou- only, the above findings remain intact. However, if twist
pling of AA stacking, Fig. 6(a), decreases the gap amplitude and displacement introduce momentum-dependent changes to
and critical temperature, it enhances these quantities in AB the electron-electron coupling interaction potentials, similar
ordering, Fig. 6(c). This finding is reversed for the interlayer to those presented in Table III, one should repeat the above
BCS coupling scenario in AA configuration. The real parts of calculations with these momentum-dependent potentials.
, f11 and f12
↑↓ ↓↑
f11 , f12 play a crucial role resulting in dramatic
↑↓ ↓↑

changes to the gap function and critical temperature. The un-


derlying reason for these changes can be understood by com- V. SUMMARY
pairing Figs. 2 and 3 with Figs. 4 and 5. The displacement
 induces real parts to f11 ↑↓ ↑↓
and f12 with interlayer and intra- In summary, using an effective Hamiltonian approach to
lyer phonon-mediated electron-electron coupling of AA and discuss in-plane displacements between graphene monolay-
AB orderings, respectively, Figs. 6(b) and 6(c). However, a ers in a bilayer graphene system, we investigate the super-
nonzero displacement  applied to AA and AB orderings with conducting pairing correlations by deriving the anomalous
11

Green’s function. Motivated by a recent experiment, we con- conducting gap function and critical temperature in a specific
sider both intralayer and interlayer phonon-mediated electron- scenario of displacement (in-plane shifting of the monolay-
electron couplings in AA and AB stacking orders. Our re- ers of graphene) in AA and AB stacking orders. We find
sults reveal that both AA and AB configurations at the charge that AA stacking with an intralayer electron-electron coupling
neutrality point, µ = 0, can only develop even-parity s-wave most favorably hosts s-wave superconductivity while AA or-
and odd-parity p-wave superconducting correlations. At a fi- dering with interlayer electron-electron coupling is the next
nite doping, µ , 0, this finding remains intact in a AA sys- desirable platform. Also, the exertion of a slight in-plane
tem with the addition of odd-parity f -wave symmetry while shift in bilayer graphene can increase both the amplitude of
AB ordering, exclusively, can host even-parity d-wave sym- the superconducting gap and critical temperature in AA and
metries. Introducing a generic coupling potential between AB orderings with phonon-mediated interlayer and intralayer
graphene monolayers in bilayer graphene, we show that dis- electron-electron couplings.
placement of graphene monolayers can induce d-wave sym-
metry at µ = 0 as well. Our results suggest that a switching to
d-wave symmetry can be achieved by a simple displacement ACKNOWLEDGMENTS
of the two coupled pristine graphene layers at a finite density
of charged carriers. We also discuss the possible appearance M.A. is supported by Iran’s National Elites Foundation
of pseudospin-triplet and odd-frequency pairings. Finally, we (INEF). Center for Nanostructured Graphene is supported
consider an s-wave interaction potential and study the super- by the Danish National Research Foundation (Project No.
DNRF103).

Appendix A: Hamiltonian of SLG with superconductivity


√ √
A monolayer graphene can be described by two valleys in k-space: K = 2π 3a (1, +1/ 3) and K = 3a (1, −1/ 3). At low ener-
0 2π

gies, the dispersion relation near the corners of the Brillouin zone, i.e., K and K0 are linear and can be described by a Dirac
Hamiltonian: HK (k) = ~vF k · σ. The corresponding wavefunction is a two-component spinor, namely,
ψAK (k) ψAK (k)
! ! !
0 k x − iky
~vF =ε . (A1)
k x + iky 0 ψBK (k) ψBK (k)
Here, A and B denote the sublattices of graphene honeycomb lattice. Note that the Hamiltonian above couples these two
sublattices. This appears because the nearest neighbor site of each sublattice site belongs to the other sublattice. This can be
clearly seen in Fig. 1(a), where sublattices are marked by blue and red colors. Hence, the total spin-less Hamiltonian can be
expressed by:
!
HK (k) 0
H(k) = , (A2)
0 HK0 (k)
where HK0 (k) = ~vF k · σ ∗ . Next, we can add spin to this Hamiltonian by introducing Pauli matrices acting in spin-space:
τ = (τ x , τy , τz ). In this case, the spin-full Hamiltonian can be expressed by Htot = H(k)τ0 where τ0 reflects the absence of spin
coupling. In SLG the two valleys are decoupled in the absence of an external potential73 . Note that the form Eq. (A2) applies
even in the presence of elastic impurities and disorder. Therefore, the Hamiltonian becomes degenerated and reduces to a 4 × 4
Hamiltonian. Now we incorporate superconductivity by introducing a two-electron amplitude,
D E
∆S ψ†A↑K ψ†B↓K0 + H.c., (A3)
in which ∆S is the gap representing BCS spin-singlet phonon-mediated electron-electron coupling between sublattices A, B and
valleys K, K0 . Note that there are several options to introduce a two-electron amplitude in the presence of superconductivity,
including Pspin-triplet coupling that couples two electrons in the same sublattice51,71,72 . In the main text, we have used the above
two-electron amplitude Eq. (A3) in our calculations. It is worth mentioning that the hole-excitation block of the Hamiltonian in
the particle-hole space, when introducing superconductivity, is equivalent to the Hamiltonian of K0 valley. Therefore, supercon-
ductivity can be viewed as a mean to introduce valley coupling in SLG. When two normal SLGs are coupled (making a BLG),
more options for incorporating the two-electron amplitudes in its superconducting phase are generated. To clarify the presence
of the second SLG, we have introduced indices 1, 2 that label top and bottom SLGs as described in the main text. In this case, to
be consistent with the previous case, we consider the following two-electron amplitude:
D E
∆B ψ†1A↑K ψ†2B↓K0 + H.c., (A4)
where ∆B is the gap representing BCS spin-singlet phonon-mediated electron-electron coupling between sublattices A, B, valleys
K, K0 , and layers 1,2. To simplify our notation throughout the presentation in the main text, due to the spin-degeneracy55–57 , we
have dropped spin and valley K, K0 indices and only keep the sublattice indices. Since we discuss AA and AB stacking orders,
from now on, we change our notation of A,B sublattices to ↑,↓ and call them pseudospin (Pspin).
12

Appendix B: Green’s function of displaced BLG with superconductivity

In this part, we present expressions derived for the anomalous Green’s function in the presence of a finite doping, considering
intralayer and interlayer phonon-mediated electron-electron couplings.

•Intralayer BCS coupling, ∆S , 0, ∆B = 0, in AA stacking order


 2    
Ω f11
↑↑
= +2∆S k− µ ∆2S + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2S − µ2 + t2 + ω2n − 3t4 − 2t2 ∆2S − µ2 + ω2n , (B1a)
        
Ω f11 ↑↓
= −∆S k−3 k+3 − k−2 k+2 −3∆2S + µ2 + t2 − 3ω2n + k− k+ ∆2S + µ2 + ω2n 3∆2S − µ2 + 3ω2n − t4 + 2t2 ∆2S + 5µ2 + ω2n +
   
∆2S + (t − µ)2 + ω2n ∆2S + µ2 + t2 + ω2n ∆2S + (µ + t)2 + ω2n , (B1b)
      
Ω f12 = −2∆S k− t ∆2S − 3µ2 + ω2n ∆2S + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2S + µ2 − t2 + ω2n + t4 + 2t2 ∆2S + µ2 + ω2n , (B1c)
↑↑
     
Ω f12↑↓
= −2∆S µt −3k−2 k+2 + 2k− k+ −∆2S + µ2 + t2 − ω2n + ∆2S + (t − µ)2 + ω2n ∆2S + (µ + t)2 + ω2n , (B1d)
         
Ω f11
↓↑
= −∆S −k−3 k+3 + k−2 k+2 −3∆2S + µ2 + t2 − 3ω2n + k− k+ − ∆2S + µ2 + ω2n 3∆2S − µ2 + 3ω2n + t4 − 2t2 ∆2S + 5µ2 + ω2n −
   
∆2S + (t − µ)2 + ω2n ∆2S + µ2 + t2 + ω2n ∆2S + (µ + t)2 + ω2n , (B1e)
  2     
Ω f11
↓↓
= −2∆S k+ µ ∆2S + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2S − µ2 + t2 + ω2n − 3t4 − 2t2 ∆2S − µ2 + ω2n , (B1f)
      
Ω f12↓↑
= +2∆S µt −3k−2 k+2 + 2k− k+ −∆2S + µ2 + t2 − ω2n + ∆2S + (t − µ)2 + ω2n ∆2S + (µ + t)2 + ω2n , (B1g)
      
Ω f12 = +2∆S k+ t ∆2S − 3µ2 + ω2n ∆2S + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2S + µ2 − t2 + ω2n + t4 + 2t2 ∆2S + µ2 + ω2n , (B1h)
↓↓
    2      2 
Ω = k−2 k+2 + 2k− k+ ∆2S − (t − µ)2 + ω2n + ∆2S + (t − µ)2 + ω2n k−2 k+2 − 2k− k+ −∆2S + (µ + t)2 − ω2n + ∆2S + (µ + t)2 + ω2n (B1i)
,

•Intralayer BCS coupling, ∆S , 0, ∆B = 0, in AB stacking order


    2  
Ω f11↑↑
= +2∆S µ k−3 k+2 + 2k−2 k+ ∆2S − µ2 + ω2n + k− ∆2S + µ2 + ω2n − k+ t2 µ2 + ω2n , (B2a)
          
Ω f11
↑↓
= −∆S k−3 k+3 + k−2 k+2 3∆2S − µ2 + 3ω2n + k− k+ ∆2S + µ2 + ω2n 3∆2S − µ2 + 3ω2n + t2 µ2 + ω2n − 2iµt2 ωn ∆2S + k+2 + µ2 −
      2      
2k+2 µ2 t2 + ω4n 3 ∆2S + µ2 + t2 + ω2n 3 ∆2S + µ2 + ∆2S t2 − 2iµt2 ω3n + ∆2S + µ2 ∆2S + µ(µ − t) ∆2S + µ(µ + t) + ω6n ,(B2b)
      
Ω f12↑↑
= −∆S t −2k−3 k+ µ + k−2 2µ −∆2S + (µ + iωn )2 + k+2 (µ + iωn ) + 2ik− k+ ωn ∆2S + µ2 + ω2n −
  
(µ − iωn ) ∆2S + µ2 − t(µ + iωn ) + ω2n ∆2S + µ(µ + t) + itωn + ω2n , (B2c)
    
Ω f12↑↓
= +2∆S µt −k−2 k+ (µ − iωn ) + k− (µ + iωn ) ∆2S + k+2 + µ2 + ω2n − k+ (µ − iωn ) ∆2S + µ2 + ω2n , (B2d)
         
Ω f11 = −∆S −k− k+ + k− k+ −3∆S + µ − 3ωn − k− k+ ∆S + µ + ωn 3∆S − µ + 3ωn + t µ + ωn − 2iµt ωn ∆S + k+ + µ2
↓↑ 3 3 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2 2

      2      
+2k+2 µ2 t2 − ω4n 3 ∆2S + µ2 + t2 − ω2n 3 ∆2S + µ2 + ∆2S t2 − 2iµt2 ω3n − ∆2S + µ2 ∆2S + µ(µ − t) ∆2S + µ(µ + t) − ω6n (B2e) ,
        
Ω f11↓↓
= −2∆S µ k−2 k+3 + k− k+2 2 ∆2S − µ2 + ω2n + t2 + ∆2S k− t2 − k+3 t2 − k+ ∆2S + µ2 + ω2n −∆2S − µ2 + t2 − ω2n , (B2f)
     2

Ω f12↓↑
= −∆S t 2iµωn (k− + k+ ) ∆2S + k− k+ + µ2 + 2iµω3n (k− + k+ ) + (k+ − k− ) ∆2S + k− k+ − µ4 + µ2 t2 −
  
ω2n (k− − k+ ) 2∆2S + 2k− k+ + t2 + ω4n (k+ − k− ) , (B2g)
     
Ω f12↓↓
= −∆S t k−2 k+2 (µ − iωn ) − 2k− k+ k+2 µ + iωn ∆2S + µ2 + ω2n − 2k+2 µ ∆2S − (µ − iωn )2 −
  
(µ + iωn ) ∆2S + µ(µ + t) − itωn + ω2n ∆2S + µ2 − µt + itωn + ω2n , (B2h)
        
Ω = ∆8S + 4∆6S µ2 + ω2n + k−4 k+4 + 4k−3 k+3 ∆2S − µ2 + ω2n + 2k−2 k+2 3∆4S − 2∆2S µ2 + 3µ4 + ω2n 6∆2S − 2µ2 + t2 − µ2 t2 + 3ω4n
    2     3  
−2∆2S µ2 t2 + 4k− k+ ∆2S + µ2 + ω2n ∆2S + ω2n − µ4 + t2 µ2 + ω2n + 4∆2S −k+2 µ2 t2 + µ2 + ω2n + t2 ω4n − µ4
  2    2   
+ 2∆4S 3 µ2 + ω2n + t2 ω2n − µ2 + µ2 + ω2n (t − µ)2 + ω2n (µ + t)2 + ω2n , (B2i)
13

•Interlayer BCS coupling, ∆S = 0, ∆B , 0, in AA stacking order

 
Ω f11↑↑
= 8i∆B k− µtωn ∆2B + k− k+ + µ2 − t2 + ω2n , (B3a)
       2

Ω f11
↑↓
= 2i∆B tωn k−2 k+2 + 2k− k+ ∆2B + 3µ2 − t2 + ω2n + 2ω2n ∆2B + µ2 + t2 + ∆2B + µ2 − t2 + ω4n , (B3b)
  2     
Ω f12
↑↑
= 2∆B k− µ ∆2B + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2B − µ2 − t2 + ω2n + t4 − 2t2 ∆2B + µ2 + 3ω2n , (B3c)
         2

Ω f12
↑↓
= −∆B ∆2B + k− k+ + µ2 − t2 + ω2n k−2 k+2 + 2k− k+ ∆2B − µ2 − t2 + ω2n + 2ω2n ∆2B + µ2 + t2 + ∆2B + µ2 − t2 + ω4n(B3d) ,
       2

Ω f11
↓↑
= 2i∆B tωn k−2 k+2 + 2k− k+ ∆2B + 3µ2 − t2 + ω2n + 2ω2n ∆2B + µ2 + t2 + ∆2B + µ2 − t2 + ω4n , (B3e)
 
Ω f11↓↓
= −8i∆B k+ µtωn ∆2B + k− k+ + µ2 − t2 + ω2n , (B3f)
         2

Ω f12
↓↑
= ∆B ∆2B + k− k+ + µ2 − t2 + ω2n k−2 k+2 + 2k− k+ ∆2B − µ2 − t2 + ω2n + 2ω2n ∆2B + µ2 + t2 + ∆2B + µ2 − t2 + ω4n (B3g) ,
  2     
Ω f12
↓↓
= −2∆B k+ µ ∆2B + µ2 + ω2n + k−2 k+2 + 2k− k+ ∆2B − µ2 − t2 + ω2n + t4 − 2t2 ∆2B + µ2 + 3ω2n , (B3h)
     
Ω = k−4 k+4 + 4k−3 k+3 ∆2B − µ2 − t2 + ω2n + 2k−2 k+2 3∆4B − 2∆2B µ2 + 3µ4 + 3t4 − 2ω2n −3∆2B + µ2 + t2 − 6∆2B t2 + 2µ2 t2 + 3ω4n
  2     
+ 4k− k+ ∆2B − µ2 + ω2n ∆2B + µ2 + ω2n − t6 + t4 3∆2B + µ2 − ω2n + t2 −3∆4B − 2∆2B µ2 + ω2n +
     2 2
µ4 + 10µ2 ω2n + ω4n + 2ω2n ∆2B + µ2 + t2 + ∆2B + µ2 − t2 + ω4n , (B3i)

•Interlayer BCS coupling, ∆S = 0, ∆B , 0, in AB stacking order

 2 
Ω f11↑↑
= −2∆B µt ∆2B + µ2 + ω2n − k−2 k+2 , (B4a)
     
Ω f11
↑↓
= −∆B k+ t k−2 k+2 + 2k− k+ ∆2B + µ2 + ω2n + ∆2B + µ2 + ω2n ∆2B − 3µ2 + t2 + ω2n , (B4b)
 2    
Ω f12
↑↑
= 2∆B k− µ ∆2B + µ2 + ω2n + k−2 k+2 + k− k+ 2 ∆2B − µ2 + ω2n + t2 , (B4c)
      
Ω f12
↑↓
= −∆B ∆2B + k− k+ + µ2 + ω2n k−2 k+2 + 2k− k+ ∆2B − µ2 + ω2n + ∆2B + µ2 + ω2n ∆2B + µ2 + t2 + ω2n , (B4d)
     
Ω f11
↓↑
= ∆B k+ t k−2 k+2 + 2k− k+ ∆2B + µ2 + ω2n + ∆2B + µ2 + ω2n ∆2B − 3µ2 + t2 + ω2n , (B4e)
   
Ω f11
↓↓
= −2∆B k+2 µt 2 ∆2B − µ2 + ω2n + 2k− k+ + t2 , (B4f)
     
Ω f12↓↑
= ∆B k−3 k+3 + k−2 k+2 3∆2B − µ2 + t2 + 3ω2n + k− k+ ∆2B + µ2 + ω2n 3∆2B − µ2 + 3t2 + 3ω2n +
   
∆2B + µ2 + ω2n ∆2B + (t − µ)2 + ω2n ∆2B + (µ + t)2 + ω2n , (B4g)
 2    
Ω f12
↓↓
= −2∆B k+ µ ∆2B + µ2 + ω2n + k−2 k+2 + k− k+ 2 ∆2B − µ2 + ω2n + t2 , (B4h)
       
Ω = k−4 k+4 + 4k−3 k+3 ∆2B − µ2 + ω2n + 2k−2 k+2 3∆4B − 2∆2B µ2 − 3ω2n + 3µ4 − 2µ2 ω2n + t2 ∆2B − µ2 + ω2n + 3ω4n +
 2    2   
4k− k+ ∆2B + µ2 + ω2n ∆2B − µ2 + t2 + ω2n + ∆2B + µ2 + ω2n ∆2B + (t − µ)2 + ω2n ∆2B + (µ + t)2 + ω2n , (B4i)
14

•Intralayer and interlayer BCS coupling, ∆S , 0, ∆B , 0, with a generic coupling matrix

Ω f11
↑↑
= 0, (B5a)
 
Ω f11
↑↓
= −∆2B ∆S − ∆B (k−− t21 + k+− t12 + iωn (t11 + t22 )) − ∆S ∆2S + k−− k+− + t11 t22 − t12 t21 + ω2n , (B5b)
Ω f12↑↑
= −(∆S k−+ t22 − ∆B t21

t22 + ∆S k−− t22

+ ∆B t12 t22

+ i(∆B (−k−− + k−+ ) + ∆S (t12 + t21∗
))ωn ), (B5c)
+ + −
Ω f12 = −(∆B + ∆S (−k− t21 + k+ t21 − i(t11 − t22 )ωn ) + ∆B (∆S + k− k+ + t21 t21 − t11 t22 + ω2n )),
↑↓ 3 − ∗ ∗ 2 ∗ ∗
(B5d)
Ω f11
↓↑
= ∆2B ∆S + ∆B (k+− t12 + k−− t21 + i(t11 + t22 )ωn ) + ∆S (∆2S + k−− k+− − t12 t21 + T 1t22 + ω2n ), (B5e)
Ω f11
↓↓
= 0, (B5f)
Ω f12↓↑
= ∆3B + ∆S (−k++ t12 + k−− t12 ∗
+ i(t11

− t22 )ωn ) + ∆B (∆2S + k−− k++ + t12 t12 ∗
− t11∗
t22 + ω2n ), (B5g)
+ +
Ω f12 = ∆S k+ t11 + ∆S k+ t11 − ∆B t11 t12 + ∆B t11 t21 + i(∆B (−k+ + k+ ) + ∆S (t12 + t21 ))ωn ,
↓↓ − ∗ ∗ ∗ − ∗
(B5h)
− + − + − + ∗ − + + ∗ +
Ω = ∆B + ∆S + k− k− k+ k+ − k− k− t12 t21 − k+ k+ t12 t21 + t12 t12 t21 t21 + ∆B ∆S ((k− − k− )(t12 + t21 ) + (k+ − k+ )(t12 + t21 )) −
4 4 ∗ ∗ ∗ − − ∗

k−+ k+− t11


∗ ∗ ∗
t22 − t11 t12 t21 t22 − k−− k++ t11 t22
∗ ∗
− t11 ∗
t12 t21 t22 + t11 t11
∗ ∗
t22 t22 − i(k+− t11

t12 + k−− t11 t12

+ k−+ t11

t21 + k++ t11 t21

+ k−+ t12

t22 +
+ + + + − − +
k+ t21 t22 + k+ t12 t22 + k− t21 t22 )ωn + (k− k+ + k− k+ + t11 t11 + t12 t12 + t21 t21 + t22 t22 )ωn + ωn + ∆B (2∆S + k− k+ + k− k+ +
− ∗ ∗ − ∗ − − ∗ ∗ ∗ ∗ 2 4 2 2


t12 t12 + t21 t21
∗ ∗
− t11 ∗
t22 − t11 t22 + 2ω2n ) + ∆2S (k−− k+− + k−+ k++ − t12 t21 − t12 ∗ ∗
t21 + t11 t22 + t11 t22 + 2ω2n ).
∗ ∗
(B5i)
Here we have defined k±+ = k cos(θk + θ/2) ± ik sin(θk + θ/2) and k±− = k cos(θk − θ/2) ± ik sin(θk − θ/2) according to the main
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