Experimental electronic structure of the electrically switchable antiferromagnet CuMnAs A. Garrison Linn1Peipei Hao1Kyle N. Gordon1Dushyant Narayan1Bryan S. Berggren1Nathaniel

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Experimental electronic structure of the electrically switchable antiferromagnet

CuMnAs

A. Garrison Linn,1, ∗Peipei Hao,1Kyle N. Gordon,1Dushyant Narayan,1Bryan S. Berggren,1Nathaniel

Speiser,1Sonka Reimers,2, 3 Richard P. Campion,2V´ıt Nov´ak,4Sarnjeet S. Dhesi,3Timur Kim,3Cephise

Cacho,3Libor ˇ

Smejkal,4, 5 Tom´aˇs Jungwirth,2, 4 Jonathan D. Denlinger,6Peter Wadley,2and Dan Dessau1, 7

1Department of Physics, University of Colorado at Boulder, Boulder, CO 80309, USA

2School of Physics and Astronomy, University of Nottingham,

University Park, Nottingham NG7 2RD, United Kingdom

3Diamond Light Source, Harwell Science and Innovation Campus, Didcot OX11 0DE, United Kingdom

4Institute of Physics, Academy of Sciences of the Czech Republic,

Cukrovarnicka 10, 162 00 Praha 6, Czech Republic

5Institut f¨ur Physik, Johannes Gutenberg-Universit¨at of Mainz, 55128 Mainz, Deutschland

6Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

7Center for Experiments on Quantum Materials, Boulder, CO 80309, USA

(Dated: October 11, 2022)

Tetragonal CuMnAs is a room temperature antiferromagnet with an electrically reorientable

N´eel vector and a Dirac semimetal candidate. Direct measurements of the electronic structure of

single-crystalline thin ﬁlms of tetragonal CuMnAs using angle-resolved photoemission spectroscopy

(ARPES) are reported, including Fermi surfaces (FS) and energy-wavevector dispersions. After cor-

recting for a chemical potential shift of ≈ −390 meV (hole doping), there is excellent agreement of

FS, orbital character of bands, and Fermi velocities between the experiment and density functional

theory calculations. Additionally, 2x1 surface reconstructions are found in the low energy electron

diﬀraction (LEED) and ARPES. This work underscores the need to control the chemical potential

in tetragonal CuMnAs to enable the exploration and exploitation of the Dirac fermions with tunable

masses, which are predicted to be above the chemical potential in the present samples.

CuMnAs has emerged as an exciting material, both

for spintronic applications [1, 2] and the study of anti-

ferromagnetic (AFM) Dirac materials [3–5]. CuMnAs

has a combined inversion and time reversal symmetry,

PT , that connects two oppositely oriented magnetic

Mn sublattices with a N´eel temperature ∼480 K [see

Fig. 1(a)] [6, 7]. This PT symmetry, highlighted in

Fig. 1(a), in conjunction with the relativistic spin-orbit

coupling allows a current to induce a non-equilibrium

spin-polarization that is staggered and commensurate

with the equilibrium AFM order. The non-equilibrium

and equilibrium AFM moments couple to each other re-

sulting in a spin orbit torque that reorients the N´eel

vector. Therefore, current driven through CuMnAs can

eﬃciently reorient the N´eel vector. This was theoret-

ically predicted [5, 8] and experimentally conﬁrmed in

CuMnAs and in another PT symmetric antiferromagnet,

Mn2Au [1, 9–11]. For example, photoemission electron

microscopy with x-ray magnetic linear dichroism provid-

ing contrast was used to directly image the N´eel vector

reorientation after passing currents through tetragonal

CuMnAs [9].

Control over the N´eel vector allows manipulation of

some electronic properties of CuMnAs. First, the pres-

ence of magnetic order gives rise to an anisotropic magne-

toresistance (AMR). Therefore, the resistivity along the

∗Corresponding Author: Garrison.Linn@colorado.edu

alattice direction can be modulated by orienting the N´eel

vector to be perpendicular or parallel to a, for example.

Wadley et al. made such a device out of a thin ﬁlm of

tetragonal CuMnAs and used the AMR signal to demon-

strate the electrical switching of the N´eel vector [1]. The

electrical switching was even shown to be scalable to THz

speeds [10]. Second, the PT symmetry provides doubly

degenerate bands, which allows for the existence of an-

tiferromagnetic Dirac fermions close to or at the Fermi

level [5]. Additional oﬀ-centered or nonsymmorphic crys-

tallographic symmetries can protect the massless Dirac

fermions. The presence or absence of these symmetries

can be controlled by reorienting the N´eel vector result-

ing in tunable masses of the Dirac fermions. The opening

and closing of the Dirac mass gap results in enhancement

of the AMR[5, 11].

Both the tetragonal and orthorhombic phases of CuM-

nAs have been studied theoretically and experimentally.

All of the above interesting properties are believed to be

present in both structural phases. Additionally, the or-

thorhombic phase is proposed to host a new topological

metal-insulator transition, due to the predicted presence

of a bulk Dirac point at EFand lack of other bands

crossing EF[5].

Density Functional Theory (DFT) has been critical to

the development of the above theoretical predictions, but

it has only been experimentally tested to a limited extent

in tetragonal CuMnAs: the AC permittivity (determined

from ellipsometry) and UV photoemission spectroscopy

arXiv:2210.03818v1 [cond-mat.mtrl-sci] 7 Oct 2022

were studied [12]; neutron diﬀraction and x-ray magnetic

linear dichroism were used to study the magnetic order-

ing [13]; and, more recently, experiments using scanning

tunneling microscopy elucidated the surface termination

of thin ﬁlms of tetragonal CuMnAs, discovering the exis-

tence of As step edges which may host surface reconstruc-

tions [14]. These experiments were compared to DFT

predictions; however, there exist no direct comparisons

to the band structure calculated from DFT.

Therefore, to directly probe the band structure of

CuMnAs, high resolution ARPES measurements were

made at the MERLIN ARPES endstation of beamline

4.0.3 at the Advanced Light Source and at the HR-

ARPES branch of beamline i05 at the Diamond Light

Source. The base pressure was .5×10−11 Torr, with

temperatures below 50K. Samples were 45 nm thick ﬁlms

of single-crystalline tetragonal CuMnAs with the (001)

face exposed and grown on GaP(001). The ﬁlms were

capped with 30 nm of As to protect the surfaces from con-

tamination from the ambient environment. Decapping

was performed in an environment with pressures .10−8

Torr, reaching a max temperature reading of 340 ◦C on

a pyrometer, emissivity = 0.1.

After decapping, LEED was performed in situ, re-

vealing a well ordered surface with reconstructions [see

Fig. 1(c&d)]. The (001) surface of tetragonal CuM-

nAs should produce a square reciprocal lattice with edge

lengths of 2π/a, where ais determined from XRD to

be 3.85 

A. This is seen in the LEED patterns; how-

ever, there are additional spots at the midpoints along

the edges of the squares, suggesting the presence of 2x1

and 1x2 surface reconstruction domains. The reconstruc-

tion is conﬁrmed by observing that the ﬁrst order Bragg

peaks occur at a radius of 2π/2a, where without a re-

construction they would occur at 2π/a [see Fig. 1(c)].

Despite the surface reconstruction, the LEED pattern is

sharp, indicating a successful decap. Samples were sub-

sequently transferred into the ARPES chamber, main-

taining an ultra-high vacuum environment from decap to

ARPES data acquisition.

We show the crystallographic and magnetic struc-

ture of tetragonal phase of CuMnAs in Fig. 1(a). The

nonmagnetic space group is nonsymmoprhic (P4/nmm).

Since the magnetic Mn atoms are light, the eﬀects of spin-

orbit coupling on the band-structure are highly pertur-

bative and smaller than our resolution can detect, unlike

in strongly relativistic PT antiferromagnet Mn2Au [15].

Therefore, in the antiferromagnetic state the nonrela-

tivsitic spin group (P14/2n2m2m) describes the main

energy scales of our measured band structure, includ-

ing Fermi surfaces [16]. However, within ∼10 meV of

a Dirac point, the fermion masses are required to accu-

rately describe the electronic dispersion, and to calculate

the Dirac fermion masses, spin-orbit coupling must be

included and the relativistic magnetic symmetry group

(Pm’mn) with generators {C2x|1

200},{My|01

20}, and PT

must be employed.

To model the electronic structure of tetragonal CuM-

nAs, DFT was performed, using the Generalized Gradi-

ent Approximations (GGA) with the Coulomb interac-

tion Uapplied to the Mn 3d orbitals within the Dudarev

approximation [17] [see Sec. I of Supplemental Materials

(SM) for a complete description of our DFT]. For the

reasons stated above, spin-orbit coupling was turned oﬀ

for all DFT shown, except Fig. 3(g,h,&i) and Fig. S2 in

SM. The best quantitative agreement of Fermi velocities

was found for U= 2.25 eV, while maintaining excellent

overall qualitative agreement. It was necessary to ap-

ply ≈390 meV of rigid hole doping to the chemical po-

tential from theory, i.e. the experimental Fermi energy

was found to be equal to the theoretical Fermi energy

−390 meV. Possible origins of the energy shift will be

discussed. Therefore, unless explicitly discussed, all of

the DFT shown in this manuscript has been plotted af-

ter applying the above mentioned rigid chemical potential

shift.

As a ﬁrst step to understanding the electronic struc-

ture of tetragonal CuMnAs, the in-plane Fermi surface

was measured at kz≈0 [see Fig. 2(a)] and kz≈π/c [see

Fig. 2(b)], which may be selected by tuning the photon

energy (see Sec. IV of SM). In this case, the zone center

data were taken with 85 eV photons, whereas the zone

edge data were taken at 100 eV. In both cases, the Fermi

surface shows strong agreement with the DFT—they

both show a propeller-shaped Fermi surface in the kz≈0

plane and ellipses at the Rpoints in the kz≈π/c plane,

with the experiment and theory displaying a very sim-

ilar shape and size of these features [see Fig. 2(c) and

Fig. 2(d)]. There are, however, three subtle eﬀects that

might naively appear as qualitative discrepancies be-

tween the experiment and theory: First, unlike the DFT,

the data shown in Fig. 2(b&d) does not have C4symme-

try. While turning on spin-orbit coupling in the DFT

would break this symmetry, the aﬀect is too small to

explain the data or even detect (see Fig. S2 of SM for

Fermi surfaces with spin-orbit coupling included). In-

stead, it is primarily the transition matrix element that

is known to modulate the ARPES spectral intensity that

is responsible for breaking the C4symmetry in the data.

In fact, a detailed analysis of this matrix element eﬀect

reveals the orbital character of the Fermi surface, which

is in good agreement with that of the DFT (see Sec. V

of SM). Second, due to the inherent surface sensitivity

of ARPES and lack of translational symmetry perpen-

dicular to the surface, ARPES spectra from any photon

energy can contain contributions from multiple kzval-

ues. This explains the closed ellipses near the Xpoints

in Fig. 2(a) and some of the weight at kx= 0 near the

Zpoint in Fig. 2(b). This point is visually illustrated in

Fig. 2(c) by overlaying the DFT from a second kzvalue

(orange transparency) that is 0.35π/c away from the an-

ticipated kzvalue (red transparency). Third, there is

extra spectral weight near the Zpoint in Fig. 2(d) indi-

cated by white text, which is identiﬁed as a replica of the

vertical ellipses enclosing the zone edges at kx= 0. The

back-folding of this ellipse onto Zis the analogue of the

2x1 surface reconstructions observed in the LEED and

will be analyzed quantitatively later.

To clearly illustrate that the DFT must be hole doped

to be consistent with the experimental data, the undoped

and doped Fermi surface from the DFT are shown in

Fig. 2(e) and Fig. 2(f), respectively. First, the experi-

mental Fermi surface does not show pockets near the M

points. Second, the pocket near the Γ point clearly con-

nects with the pocket near the Xpoint in the experimen-

tal data. These points are inconsistent with the undoped

Fermi surface. However, after lowering the chemical po-

tential of the DFT by ≈0.390 eV (rigid hole doping), all

of the qualitative and even quantitative features of the

experimental Fermi surface are consistent with the bulk

DFT calculations.

With the aid of Fermi surface plots and kzdisper-

sion (see Sec. IV of SM IV), E-kdispersion for the

high symmetry cuts in the Γ-Xplane are readily ac-

quired using 85 eV, LV polarized photons. To quantita-

tively compare the experimental data to DFT, momen-

tum distribution cuts (MDCs) are ﬁt to extract the low

energy experimental dispersion, including Fermi veloci-

ties [see Fig. 3(a-f)]. The X→Γ→XMDCs are ﬁt

with two Voigt functions, and the extracted Fermi veloc-

ity is 4.6 eV 

A, which to within the experimental error

bars is the same as the Fermi velocity from the DFT,

vF= 4.8 eV 

A. The M→X→Msymmetry cut con-

tains the A→R→Abands near EF, due to the same kz

uncertainty mentioned above. Therefore, the extracted

MDCs were ﬁt with four Voigt functions, representing

four bands. The Fermi velocity of the bands correspond-

ing to the M→X→Mcut is 6.0 eV 

A. Again to within

experimental precision, this is the same as the Fermi ve-

locity from the DFT, vF= 6.4 eV 

A. The error on the

extracted Fermi velocities from MDC ﬁttings scales as

∼vF2. So, for these large Fermi velocities, the relative

error is found to be ∼10% (see Sec. VII of SM). To see

the full ARPES images for several high symmetry cuts

along with a matrix element analysis of the cuts shown,

see Sec. VI of SM.

The strong agreement between the DFT and experi-

ment shown throughout this paper lend credence to the

predictions from the DFT beyond the ones directly ver-

iﬁed. For example, this applies to the atomic charac-

ter of the bands predicted by the DFT [see Fig. S1 of

SM]. More importantly, the DFT predicts the presence

of Dirac fermions with a tunable mass gap, which are

present in the DFT when spin-orbit coupling is included

[see Fig. 3(g-i)]. The closest of which is just 180 meV

above the stoichiometric and defect free Fermi energy.

Note that moving EFto this Dirac point should enable

band topology switching.

Having demonstrated the strong agreement between

the DFT and experiment, it is time to address two issues

raised previously in detail—the replication and doping.

First, to quantitatively test the hypothesis that the ex-

tra structure near the Zpoint of the Fermi surface is the

replication of the ellipses near the Rpoint [see Fig. 4(a)],

the dispersion along the R→Z→Rcut is compared

to the dispersion along the A→R→Acut. MDC ﬁt-

ting is used to extract the experimental dispersion along

the R→Z→Rcut [see Fig. 4(b)]. The MDCs are ﬁt

with three Voigt functions—two to capture the bands in

question and one to capture a band top at kx= 0 that

disperses across EFas a function of kz. The extracted

dispersion from the R→Z→Rcut is overlaid with

the DFT dispersion along the A→R→Acut, show-

ing excellent qualitative agreement [see Fig. 4(c)]. From

MDC analysis, the Fermi velocity of the bands in the

R→Z→Rcut is determined to be 5.1 eV 

A. The

Fermi velocity of the A→R→Acut extracted from the

DFT is 5.2 eV 

A, which is within 2% of the experimental

value.

Second, to determine if the ≈390 meV chemical poten-

tial shift is reasonable, necessary concentrations of likely

defects are calculated. It turns out that two eﬀects al-

low this relatively large energy shift to be explained by

reasonably small defect concentrations. First, CuMnAs

is a semimetal. According to the DFT, ≈390 meV of

hole doping corresponds to only 0.27 holes per unit cell.

Second, the most likely defects all bring a substantial

number of holes with each defect. According to M´aca et

al., the most energetically favorable defects are Cu and

Mn vacancies followed by Mn substitutions for Cu [18].

One reasonably suspects that the non-magnetic copper

will have 10 valence electrons, i.e. will be [Ar] 3d10, and

the magnetic Mn will be [Ar] 3d5with 5 valence elec-

trons, naively leaving As with a full valence shell. The

atomically projected Density Of States (DOS) from the

DFT mostly agrees with this intuition, ﬁnding 10 valence

electrons on Cu and 5.4 on Mn, which would mean that

each Mn for Cu substitution brings 4.6 holes. Therefore,

taking into account the 222 stoichiometry of the unit cell,

the 388 meV shift would result from only 1.3%, 2.4%, and

2.9% of pure Cu or Mn vacancies or Mn for Cu substitu-

tions, respectively. Furthermore, there could be combi-

nations of these defects, yielding very reasonable defect

levels. Speciﬁcally, the defect concentrations in the few

percent range give, according to M´aca at al. [18], DFT

resistivities of CuMnAs consistent with experiment.

In-plane Fermi surfaces, kzdispersions (see Sec. IV of

SM), and symmetry cuts as E-kdispersions for tetrago-

nal CuMnAs are reported for the ﬁrst time. After shift-

ing the chemical potential by ≈ −390 meV (hole doping),

DFT calculations—using GGA+U with U= 2.25 eV ap-

plied to the Mn-3d orbitals—are found to be in excellent

qualitative and quantitative agreement with the experi-

mental data. In particular, the DFT predicts accurate

Fermi velocities and an orbital character for the bands

that is consistent with the experimental results. Addi-

tionally, surface reconstruction and replicated bands are

found.

Furthermore, the extracted value of Uis consistent

with that of other studies. Veis et al. found that

Ueff = (U−J)≈2 eV ﬁt their angle-integrated pho-

toemission data best [12]. In the GGA+U scheme used

for the calculations in this paper, Uand Jvalues are

not separate, and what really enters the total energy is

the “U−J” value. So, the U= 2.25 eV term in this

manuscript corresponds to the Ueff . Guyen et al. used

U= 2 eV to explain emergent edge states on their surface

reconstructed CuMnAs thin ﬁlms [14]. U < 2 eV fails to

even qualitatively capture the ARPES experimental re-

sults, primarily because the bandwidth of the band in the

X→Γ→Xis too small. The strongly constrained and

appropriately normed (SCAN) functional [19] increased

this bandwidth compared to pure GGA, yielding a similar

bandwidth to U= 1 eV. Nevertheless, SCAN still did not

produce a large enough bandwidth for the X→Γ→X

cut. U= 2.25 eV within GGA was primarily chosen be-

cause it reproduces the Fermi velocity in the X→Γ→X

cut most accurately.

By showing that DFT accurately captures the elec-

tronic structure of tetragonal CuMnAs, more weight is

given to the growing interest in CuMnAs as a candidate

AFM topological Dirac material. Furthermore, the low

DOS near EFprovides hope that tetragonal CuMnAs

can be electron doped moving EFinto the proximity of

the electrically switchable Dirac points above EFin the

studied ﬁlms. According to the DFT, the Dirac points are

570 meV or ∼0.38 electrons per unit cell above the chem-

ical potential in the current ﬁlms or only 180 meV/∼0.12

electrons per unit cell above the defect free chemical po-

tential. Alternatively, orthorhombic CuMnAs was sug-

gested to be a pristine antiferromagnetic Dirac semimetal

with only Dirac fermions at the Fermi level without any

trivial bands. Considering the reliability of DFT in the

description of tetragonal CuMnAs presented here, study-

ing orthorhombic CuMnAs appears as a promising direc-

tion in research of antiferromagnetic Dirac semimetals.

A. G. Linn and K. N. Gordon contributed equally to

gathering the ARPES data with support from J. D. Den-

linger, P. Hao, B. S. Berggren, D. Narayan, T. Kim, C.

Cacho, N. Speiser, S. Reimers, and S. Dhesi. The DFT

shown in this paper was performed by P. Hao with feed-

back from A. G. Linn, D. Dessau, L. ˇ

Smejkal, and T.

Jungwirth. P. Wadley oversaw the growth and charac-

terization of the thin ﬁlms of tetragonal CuMnAs by R.P.

Campion and V. Novak. This manuscript was prepared

by A. G. Linn under guidance from Dan Dessau and with

feedback from all authors. Dan Dessau was the principal

investigator overseeing the work.

This work was supported by DOE grant DE-FG02-

03ER46066, Betty and Gordon Moore Foundation grant

GBMF9458, Ministry of Education of the Czech Republic

Grants LNSM-LNSpin, LM2018140, Czech Science Foun-

dation Grant No. 19-28375X, and EU FET Open RIA

Grant No. 766566. Additionally, P.Wadley acknowledges

support from the Royal Society through a Royal Society

University Research Fellowship. This research used re-

sources of the Advanced Light Source, a U.S. DOE Oﬃce

of Science User Facility under contract no. DE-AC02-

05CH11231. We would like to thank the Diamond i05

ARPES (SI22665, SI24224-1) and ALS Merlin ARPES

end station teams for allowing us time for and aiding in

the ARPES data acquisition.

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ExperimentalelectronicstructureoftheelectricallyswitchableantiferromagnetCuMnAsA.GarrisonLinn,1,PeipeiHao,1KyleN.Gordon,1DushyantNarayan,1BryanS.Berggren,1NathanielSpeiser,1SonkaReimers,2,3RichardP.Campion,2VtNovak,4SarnjeetS.Dhesi,3TimurKim,3CephiseCacho,3LiborSmejkal,4,5TomasJungwirth,2,4Jo...

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Experimental electronic structure of the electrically switchable antiferromagnet CuMnAs A. Garrison Linn1Peipei Hao1Kyle N. Gordon1Dushyant Narayan1Bryan S. Berggren1Nathaniel

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