Supplemental Material for Antiferromagnetism in the van der Waals layered spin-lozenge

semiconductor CrTe3

Michael A. McGuire,1 V. Ovidiu Garlea,2 Santosh KC,1 Valentino R. Cooper,1 Jiaqiang Yan,1 Huibo Cao,2 and Brian C. Sales1
1
Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831 USA
2
Quantum Condensed Matter Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831 USA

SUPPLEMENTARY MATERIAL tion at 10 K.

Magnetic susceptibility vs temperature for two polycrys-
talline samples of CrTe3 is shown in Fig. S1. Sample 1
is relatively high purity and the data shown are from mea-
surements carried out in a field of 50 kOe. Sample 2 is less
pure, with Cr5 Te8 providing a ferromagnetic component be-
low about 280 K. For this sample the data shown were deter-
mined from linear fits to M vs H data between 30 and 50 kOe.
Rietveld fits to neutron powder diffraction data collected at
10 and 300 K are shown in Figure S2. The fitted crystallo-
graphic parameters are collected in Table S1. Low Q portions
of the data are shown in Fig. S3, in which the magnetic Bragg
peak (0.5, 1.5, -0.5) can be seen. The limited statistics of this
data make determining the ordering temperature difficult, but
the contour plot of intensity shown in the inset appears to be
consistent with the single crystal data, which showed onset of
magnetic scattering near 56 K. The relative breadth and appar-
ent asymmetry of the magnetic peak suggests that there may
be some residual magnetic disorder along the stacking direc-
The temperature dependence of the lattice parameters de-
termined from neutron and x-ray powder diffraction measure-
ments are shown in Figure S4. The largest discrepancy is seen
in a, which varies by about 0.1% between the two measure-
ments. This is expected to be due primarily to small sample
to sample variations, and it may indicate some degree of sto-
ichiometric variation in the CrTe3 phase. Values for a rang-
ing from 7.884 to 7.899 Å were observed at room temperature
based on powder x-ray diffraction measurements.
Results of single crystal x-ray diffraction refinements are
collected in Table S2, which lists lattice parameters and agree-
ment indices, as well as atomic coordinates and equivalent
isotropic displacement parameters.
The calculated total and projected densities of states for
CrTe3 are shown in Fig. S5. This calculation was performed
using the AFM2 configuration.
The positions and moments on the Cr atoms determined by
single crystal neutron diffraction refinement are listed in Table
S3.
 2

cm /mol-Cr)
3
2

-3
(10
polycrystalline 1, H = 50 kOe
1

polycrystalline 2, slope of high-

field M vs H curves

0
0 100 200 300 400

T (K)

FIG. S1. Magnetic susceptibility of two polycrystalline samples of CrTe3 .

300 POWGEN

T = 10 K
intensity (arb. units)

200

100

2 3 4 5 6 7 8 9 10
-1
Q (Å )

POWGEN

T = 300 K
intensity (arb. units)

200

2 3 4 5 6 7 8 9 10
-1
Q (Å )

FIG. S2. Rietveld fits to neutron powder diffraction data collected at 10 and 300 K.
 3

0.5 1.5 -0.5

FIG. S3. Powder neutron diffraction data showing a magnetic Bragg peak, marked by the arrow, that appears at low temperature.

TABLE S1. Lattice parameters and agreement indices for CrTe3 using space group P 21 /c, and atomic coordinates and isotropic displacement
parameters (Biso = 8π 2 Uiso , where U is the mean square atomic displacement) for CrTe3 determined from refinements of powder neutron
diffraction data collected at POWGEN.
Temperature 300 K 10 K

Unit cell dimensions a = 7.896(1) Å a = 7.880(1) Å

b = 11.214(1) Å b = 11.084(1) Å
c = 11.552(1) Å c = 11.518(1) Å
β =118.56(1) deg. β = 118.46(1) deg.

Volume 898.5(2) Å3 884.4(1) Å3

R indices (all data) Rp = 5.25, Rwp = 3.31 Rp = 4.89, Rwp = 3.26

x y z Biso
T = 10 K
Cr(1) 0.008(6) 0.503(4) 0.170(4) -0.2(3) Å2
Cr(2) 0.022(5) 0.233(3) 0.008(4) -0.2(3) Å2
Te(1) 0.201(5) 0.620(2) 0.398(3) 0.2(2) Å2
Te(2) 0.229(4) 0.599(2) 0.073(3) 0.2(2) Å2
Te(3) 0.278(3) 0.173(3) 0.433(2) 0.2(2) Å2
Te(4) 0.275(3) 0.326(3) 0.246(2) 0.2(2) Å2
Te(5) 0.291(4) 0.059(2) 0.095(3) 0.2(2) Å2
Te(6) 0.795(5) 0.386(2) 0.265(3) 0.2(2) Å2

T = 300 K
Cr(1) 0.011(7) 0.503(4) 0.175(4) 0.3(4) Å2
Cr(2) 0.022(5) 0.224(3) 0.008(4) 0.3(4) Å2
Te(1) 0.213(6) 0.618(2) 0.402(4) 0.9(3) Å2
Te(2) 0.218(5) 0.599(3) 0.069(4) 0.9(3) Å2
Te(3) 0.269(4) 0.175(3) 0.430(3) 0.9(3) Å2
Te(4) 0.271(4) 0.325(3) 0.246(3) 0.9(3) Å2
Te(5) 0.302(4) 0.057(3) 0.101(4) 0.9(3) Å2
Te(6) 0.793(5) 0.386(3) 0.265(3) 0.9(3) Å2
 4

7.90 11.25

x-ray x-ray

neutron neutron

11.20

7.89
a (Å)

b (Å)
11.15

7.88

11.10

7.87 11.05
0 50 100 150 200 250 300 0 50 100 150 200 250 300

11.56

x-ray x-ray

neutron neutron
118.6

11.55

11.54
(deg.)

118.5
c (Å)

11.53

118.4

11.52

11.51 118.3
0 50 100 150 200 250 300 0 50 100 150 200 250 300

T (K) T (K)

FIG. S4. Temperature dependence of the lattice parameters of two CrTe3 samples, one determined by x-ray powder diffraction and the other
by neutron powder diffraction.
 5

TABLE S2. Lattice parameters and agreement indices, and atomic coordinates and equivalent isotropic displacement parameters from refine-
ments of single crystal x-ray diffraction data from CrTe3 using space group P 21 /c with Mo radiation. The crystal size was approximately
0.070×0.040×0.005 mm3 .

Temperature 100(5) K 173(5) K 250(5) K

Unit cell dimensions a = 7.8762(5) Å a = 7.8798(5) Å a = 7.8833(5) Å

b = 11.0966(8) Å b = 11.1392(8) Å b = 11.1897(7) Å
c = 11.5207(10) Å c = 11.5313(10) Å c = 11.5423(9) Å
β = 118.373(5) deg. β = 118.418(4) deg. β = 118.456(5) deg.

Volume 885.94(12) Å3 890.19(12) Å3 895.15(11)Å3

R indices (all data) R1 = 0.0336, wR2 = 0.0776 R1 = 0.0352, wR2 = 0.0796 R1 = 0.0359, wR2 = 0.0781
Largest diff. peak and hole 5.780 and -2.434 e/Å3 4.592 and -2.894 e/Å3 3.510 and -2.749 e/Å3
x y z Ueq
T = 100 K
Cr(1) 0.0020(1) 0.4993(1) 0.1680(1) 0.007(1) Å2
Cr(2) 0.0223(1) 0.2297(1) 0.0078(1) 0.007(1) Å2
Te(1) 0.2039(1) 0.6206(1) 0.3993(1) 0.007(1) Å2
Te(2) 0.2363(1) 0.5918(1) 0.0761(1) 0.007(1) Å2
Te(3) 0.2755(1) 0.1683(1) 0.4355(1) 0.007(1) Å2
Te(4) 0.2759(1) 0.3273(1) 0.2461(1) 0.007(1) Å2
Te(5) 0.2956(1) 0.0561(1) 0.0957(1) 0.007(1) Å2
Te(6) 0.7997(1) 0.3799(1) 0.2687(1) 0.007(1) Å2

T = 173 K
Cr(1) 0.0022(1) 0.4991(1) 0.1686(1) 0.010(1) Å2
Cr(2) 0.0221(1) 0.2278(1) 0.0078(1) 0.010(1) Å2
Te(1) 0.2049(1) 0.6202(1) 0.3997(1) 0.010(1) Å2
Te(2) 0.2342(1) 0.5921(1) 0.0754(1) 0.010(1) Å2
Te(3) 0.2739(1) 0.1690(1) 0.4352(1) 0.010(1) Å2
Te(4) 0.2743(1) 0.3264(1) 0.2454(1) 0.010(1) Å2
Te(5) 0.2970(1) 0.0553(1) 0.0963(1) 0.011(1) Å2
Te(6) 0.7985(1) 0.3803(1) 0.2682(1) 0.011(1) Å2

T = 250 K
Cr(1) 0.0022(1) 0.4992(1) 0.1693(1) 0.014(1) Å2
Cr(2) 0.0217(1) 0.2258(1) 0.0076(1) 0.013(1) Å2
Te(1) 0.2061(1) 0.6198(1) 0.4002(1) 0.014(1) Å2
Te(2) 0.2322(1) 0.5926(1) 0.0748(1) 0.013(1) Å2
Te(3) 0.2722(1) 0.1696(1) 0.4350(1) 0.014(1) Å2
Te(4) 0.2726(1) 0.3258(1) 0.2446(1) 0.014(1) Å2
Te(5) 0.2984(1) 0.0545(1) 0.0969(1) 0.014(1) Å2
Te(6) 0.7973(1) 0.3806(1) 0.2676(1) 0.014(1) Å2

TABLE S3. Symmetry operators of Wyckoff positions and the corresponding magnetic moment configuration for the two non-equivalent Cr
atoms located inside the crystallographic unit cell. Note the components of the moment along the crystallographic axes are ma = 2.1(1),
mb = 0.7(1), and mc = 1.1(1)µB . The magnetic structure is defined by the propagation vector k=(0.5,0.5,0.5) and is described by the
magnetic space group PS 1.
Cr1 (0.008,0.503, 0.170) Cr2 (0.022, 0.233, 0.008)
(x, y, z) (ma , mb , mc ) (x, y, z) (−ma , −mb , −mc )
(−x + 1, y − 1/2, −z + 1/2) (ma , mb , mc ) (−x + 1, y + 1/2, −z + 1/2) (ma , mb , mc )
(−x + 1, −y + 1, −z + 1) (ma , mb , mc ) (−x + 1, −y + 1, −z + 1) (−ma , −mb , −mc )
(x, −y + 3/2, z + 1/2) (ma , mb , mc ) (x, −y + 1/2, z + 1/2) (ma , mb , mc )
 6

80 Total DOS
Cr (d)
60 Te (p)

Density of States [states/eV]

40
up
20

−20

−40
down
−60

−80

−6 −4 −2 0 2 4
Energy [eV]

FIG. S5. Calculated total and projected density of states (DOS) for CrTe3 in the AFM2 ordered state described in the text. The zero of the
energy indicates the Fermi level.