Supporting Information: High-throughput

DFT-based discovery of next generation

two-dimensional (2D) superconductors

Daniel Wines,∗,† Kamal Choudhary,†,‡ Adam J. Biacchi,¶ Kevin F. Garrity,† and

Francesca Tavazza†

†Material Measurement Laboratory, National Institute of Standards and Technology,

Gaithersburg, Maryland 20899, USA
‡Theiss Research, La Jolla, CA, 92037, USA
¶Physical Measurement Laboratory, National Institute of Standards and Technology,
Gaithersburg, Maryland 20899, USA

E-mail: [email protected]

The critical temperature of superconducting materials was determined using direct cur-
rent (DC) magnetometry. Samples of layered superconductors were purchased from Alfa
Aesar (FeSe, 2H-NbSe2 ) and 2D Semiconductors (2H-NbS2 and ZrSiS). Prior to analysis,
samples were crushed and ground with a mortar and pestle to a fine powder to remove
any orientation-based effects. Magnetic susceptibility measurements were carried out us-
ing a Quantum Design Physical Property Measurement System (PPMS) equipped with a
12 T superconducting magnet. The PPMS vibrating sample magnetometer (VSM) module
was employed and the chamber was evacuated to a pressure of 10 Torr (1.33 kPa) or less.
Samples were first zero field-cooled from room temperature to 2 K whereupon a magnetic
field of +0.001 T was applied. The temperature was then raised at a rate of 1 K/min and

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magnetic susceptibility was measured as a function of temperature to 50 K. A field-cooled
measurement was also collected where the temperature was lowered from 50 K to 2 K at 1
K/min. This procedure was then repeated for applied magnetic fields of +0.01 T and +0.1
T.

Table S1: q-point convergence of λ, ωlog , and Tc for selected promising 2D superconductors.

Structure q-point λ ωlog (K) Tc (K)

2H-TaS2 2x2x1 3.3 36.3 6.8
6x6x1 1.0 91.3 6.5
7x7x1 1.6 49.6 6.1
2H-NbSe2 2x2x1 2.5 46.6 7.6
3x3x1 1.4 41.0 4.5
4x4x1 0.9 115.8 6.4
6x6x1 0.8 131.1 6.7
W2 N3 2x2x1 0.7 369.3 10.6
3x3x1 1.8 102.0 13.4
4x4x1 1.4 171.7 18.7
Mg2 B4 N2 4x4x1 1.7 172.4 21.8
6x6x1 1.1 261.2 19.9
TiClO 4x9x1 2.7 56.0 9.7
6x9x1 2.8 63.8 11.1

Figure S1: Effect of different k-point and q-point selection on electron-phonon coupling
(EPC) parameters for 2D 2H-NbSe2 with respect to broadening: a) λ, b) ωlog , and c) Tc .

a) 5 H-NbSe2 b)140 H-NbSe2 c) 18 H-NbSe2

k: 12x12x1, q: 2x2x1
k: 36x36x1, q: 2x2x1
4.5 k: 12x12x1, q: 3x3x1
16
120 k: 36x36x1, q: 3x3x1
4 k: 12x12x1, q: 4x4x1
14 k: 36x36x1, q: 4x4x1
3.5 100 k: 12x12x1, q: 6x6x1
ωlog (K)

Tc (K)

3 12
λ

80
2.5
10
2 60
8
1.5
40
1 6
0.5 20
0.136 0.272 0.408 0.544 0.680 0 0.136 0.272 0.408 0.544 0.680 4
0 0.136 0.272 0.408 0.544 0.680
Broadening (eV) Broadening (eV) Broadening (eV)

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Figure S2: The effect of broadening value for a selected group of representative supercon-
ductors: a) λ, b) ωlog , c) Tc and d) the change in Tc with respect to µ∗ .

a) 5 b)250
4.5
4 200
3.5
3 ωlog (K)
λ

150
2.5
2
1.5 100

1
0.5 50
0 0.136 0.272 0.408 0.544 0.680 0 0.136 0.272 0.408 0.544 0.680
Broadening (eV) Broadening (eV)
c) 50 d) 30
Mg2B4N2
45 W2N3 TiClO
NbO2 H-NbS2 25
40 ZrBrO H-NbSe2

35 20
Tc (K)

Tc (K)

30
15
25
20 10
15
5
10
5 0
0 0.136 0.272 0.408 0.544 0.680 0 0.05 0.1 0.15 0.2 0.25
*
Broadening (eV) μ

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Table S2: Tabulated results for the 2D superconductors with a Tc above 5 K. Values for
JARVIS ID, k-point grid, q-point grid, λ, ωlog , Tc and formation energy per atom are given.

Structure JARVIS ID k-point q-point λ ωlog Tc Eform

(K) (K) (eV/atom)
Mg2 B4 N2 JVASP-153112 4x4x1 24x24x1 1.7 172.4 21.8 -0.24
W2 N 3 JVASP-153122 4x4x1 12x12x1 1.4 171.7 18.7 0.05
NbO2 JVASP-31356 5x5x1 25x25x1 1.6 144.5 17.5 -2.25
PtN2 JVASP-6634 2x2x1 14x14x1 0.8 228.1 11.9 1.59
MgB2 JVASP-153113 4x4x1 24x24x1 0.6 472.2 11.8 0.44
MoN JVASP-13586 2x2x1 26x26x1 1.1 133.7 11.2 1.90
TiClO JVASP-75097 4x9x1 12x9x1 2.7 56.0 9.6 -2.42
B2 N JVASP-79276 4x4x1 24x24x1 0.7 281.2 9.6 0.09
ZrBrO JVASP-28185 2x2x1 22x22x1 0.9 173.3 9.5 -2.39
2H-NbS2 JVASP-646 7x7x1 14x14x1 1.1 117.4 9.3 -1.03
NaSn2 S4 JVASP-6949 4x4x1 20x20x1 0.9 143.4 9.2 -0.60
Mg2 B4 C2 JVASP-153110 4x4x1 24x24x1 0.5 655.5 9.0 -0.28
Nb2 CuS4 JVASP-75063 2x2x1 14x14x1 1.5 73.1 8.6 -0.52
AuN2 JVASP-75054 6x4x1 18x32x1 1.4 80.6 8.4 0.76
Nb2 CoS4 JVASP-27853 2x2x1 24x24x1 0.9 143.2 8.3 -0.59
1T-NbS2 JVASP-5947 4x4x1 24x24x1 1.4 79.1 8.3 -1.00
χ-Borophene JVASP-153104 4x4x1 24x24x1 0.5 482.1 8.2 0.48
NbC JVASP-153115 4x4x1 24x24x1 0.8 197.9 8.1 0.34
ZrSiS JVASP-153121 2x2x1 24x24x1 0.9 128.2 7.9 -0.77
CoAs2 JVASP-6637 4x4x1 16x16x1 1.3 80.0 7.8 0.25
α-Mg2 B4 N2 JVASP-153111 4x4x1 24x24x1 1.0 104.2 7.4 0.06
B2 O JVASP-153100 4x4x1 24x24x1 4.8 33.3 7.0 -0.73
2H-TaS2 JVASP-6070 7x7x1 14x14x1 1.0 91.3 6.5 -1.06
2H-NbSe2 JVASP-655 4x4x1 12x12x1 0.9 115.8 6.4 -0.76
BaSn4 O8 JVASP-77697 3x3x1 9x9x1 1.3 64.0 6.3 -1.51
1T-NbSe2 JVASP-5899 6x6x1 18x18x1 3.3 33.6 6.3 -0.74
LaBi2 O4 JVASP-28176 2x2x1 14x14x1 1.4 58.5 6.2 -1.92
BrCY JVASP-60515 2x2x1 24x24x1 1.0 86.8 6.0 -1.18
2H-NbTe2 JVASP-153106 4x4x1 24x24x1 1.1 71.8 5.8 -0.33
TiSe JVASP-6010 4x4x1 12x12x1 1.4 51.8 5.4 -0.74
TiS2 JVASP-774 4x4x1 12x12x1 0.7 185.4 5.4 -1.33
ZrS JVASP-786 9x9x1 27x27x1 0.8 123.3 5.3 -1.39
AuSe2 JVASP-6601 4x4x1 15x15x1 2.7 29.9 5.1 0.29
VSe JVASP-77610 7x7x1 14x14x1 0.8 114.7 5.1 -0.47

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Figure S3: Phonon density of states (DOS) for selected structures with positive formation
energy: a) W2 N3 b) MgB2 c) χ-Borophene d)α-Mg2 B4 N2 .

a) b)
0.05

DOS (states/cm-1)
DOS (states/cm-1)

0.1
W2N3 MgB2
0.08 0.04

0.06 0.03

0.04 0.02

0.02 0.01

0 0
0 100 200 300 400 500 600 700 0 200 400 600 800
-1
Frequency (cm ) Frequency (cm-1)
c) d)
0.04 0.05
DOS (states/cm-1)
DOS (states/cm-1)

χ-Borophene α-Mg2B4N2
0.04
0.03

0.03
0.02
0.02

0.01
0.01

0 0
0 500 1000 1500 2000 0 500 1000 1500 2000
-1 -1
Frequency (cm ) Frequency (cm )

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Table S3: The 24 newly added structures (based on literature search) to the JARVIS
database with their corresponding JARVIS ID.

Structure JARVIS ID
Al4 CO JVASP-153098
β-Borophene JVASP-153101
χ-Borophene JVASP-153104
B2 N JVASP-153099
B2 O JVASP-153100
CaC6 JVASP-153102
CaRu2 N2 JVASP-153103
LiC6 JVASP-153109
Mg2 B4 C2 JVASP-153110
Mg2 B4 N2 JVASP-153112
α-Mg2 B4 N2 JVASP-153111
MgB2 JVASP-153113
MgBH JVASP-153114
Mo2 C JVASP-157996
NbC JVASP-153115
2H-NbTe2 JVASP-153106
1T-NbTe2 JVASP-153118
PdBi2 JVASP-153116
ScC JVASP-153117
2H-TaTe2 JVASP-153107
1T-TaTe2 JVASP-153119
W2 B3 JVASP-153120
W2 N3 JVASP-153122
ZrSiS JVASP-153121

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