1702.07310v1
1702.07310v1
M. Zahid Hasan∗ ,1, 2 Su-Yang Xu,1 Ilya Belopolski,1 and Shin-Ming Huang3, 1
1
Laboratory for Topological Quantum Matter and Spectroscopy (B7),
arXiv:1702.07310v1 [cond-mat.mtrl-sci] 23 Feb 2017
Abstract
Weyl semimetals are conductors whose low-energy bulk excitations are Weyl fermions, whereas
their surfaces possess metallic Fermi arc surface states. These Fermi arc surface states are pro-
tected by a topological invariant associated with the bulk electronic wavefunctions of the material.
Recently, it has been shown that the TaAs and NbAs classes of materials harbor such a state
of topological matter. We review the basic phenomena and experimental history of the discov-
ery of the first Weyl semimetals, starting with the observation of topological Fermi arcs and Weyl
nodes in TaAs and NbAs by angle and spin-resolved surface and bulk sensitive photoemission spec-
troscopy and continuing through magnetotransport measurements reporting the Adler-Bell-Jackiw
chiral anomaly. We hope that this article provides a useful introduction to the theory of Weyl
semimetals, a summary of recent experimental discoveries, and a guideline to future directions.
Keywords: topological phase of matter, topological insulator, quantum Hall effect, Chern num-
ber, topological invariant, topological phase transition, Weyl materials
∗
Email: [email protected]
1
I. INTRODUCTION
The rich correspondence between high-energy particle physics and low-energy condensed
matter physics has been a source of insights throughout the history of modern physics1,2 .
It has led to important breakthroughs in many aspects of fundamental physics, such as
the Planck constant and blackbody radiation, the Pauli exclusion principle and magnetism,
as well as the Anderson-Higgs mechanism and superconductivity, which in turn helped de-
velop materials with useful applications. In the past decade, the discovery of massless Dirac
fermions in graphene and on the surface of topological insulators has taken center stage
in condensed matter science and has led to novel considerations of the Dirac equation in
crystals3–11 . The Dirac equation, proposed in 1928 by Paul Dirac, represents a founda-
tional unification of quantum mechanics and special relativity in describing the nature of
the electron. Its solutions suggest three distinct forms of relativistic particles: the Dirac,
Majorana, and Weyl fermions. Only one year later, in 1929, Hermann Weyl pointed out
that the Dirac equation without mass naturally gives rise to a simpler Weyl equation,whose
solutions are associated with massless fermions of definite chirality, particles known as Weyl
fermions12 . Weyls equation was intended as a model of elementary particles, but in nearly
86 years, no candidate Weyl fermions have ever been established in high-energy experiments.
Neutrinos were once thought to be such particles but were later found to possess a small
mass. Recently, emergent, quasiparticle analogs of Weyl fermions have been discovered in
certain electronic materials that exhibit strong spinorbit coupling and topological behavior.
Just as Dirac fermions emerge as signatures of topological insulators4,6 , in certain types of
semimetals, such as tantalum or niobium arsenides, electrons behave like Weyl fermions.
In 1937, the physicist Conyers Herring considered the conditions under which electronic
states in solids have the same energy and crystal momentum even in the absence of any
particular symmetry13 . Near such accidental band touching points, the low-energy excita-
tions are described by the Weyl equation13–15 . In recent times, these touching points have
been studied theoretically in the context of topological materials and are referred to as Weyl
points, and the quasiparticles near them are the emergent Weyl fermions16–27 . In these
crystals, the quantum mechanical wave function of an electron state acquires a geometric or
Berry phase when tracing out a closed loop in momentum space. This Berry phase is identi-
cal to that acquired by an electron tracing out a closed loop in real space in the presence of
2
a magnetic monopole. In the same way that magnetic monopoles correspond to sources or
sinks of magnetic flux, a Weyl semimetal hosts momentum space monopoles that correspond
to sources or sinks of Berry curvature. These Berry curvature monopoles are precisely the
Weyl points of a Weyl semimetal. Furthermore, the chirality of the Weyl fermion corre-
sponds to the chiral charge of the Weyl point. In a Weyl semimetal, the chirality associated
with each Weyl node can be understood as a topologically protected charge, hence broaden-
ing the classification of topological phases of matter beyond insulators. Remarkably, Weyl
nodes are extremely robust against imperfections in the host crystal and are protected by
the crystal’s inherent translational invariance. The real-space Weyl points are associated
with chiral fermions, and in momentum space they behave like magnetic monopoles. The
fact that Weyl nodes are related to magnetic monopoles suggests that they will be found
in topological materials that are in the vicinity of a topological phase transition. Like a
topological insulator, a Weyl semimetal hosts topological surface states arising from a bulk
topological invariant. However, while the surface states of a topological insulator have a
Fermi surface that consists of closed curves in momentum space, a Weyl semimetal hosts
an exotic, anomalous surface-state band structure containing topological Fermi arcs, which
form open curves that terminate on bulk Weyl points17,24,25 . Theory has suggested that in
systems where inversion or time-reversal symmetry is broken, a topological insulator phase
naturally allows a phase transition to a Weyl semimetal phase. Building on these ideas, many
researchers, including the Princeton University group, used ab initio calculations to predict
candidate materials and perform angle-resolved photoemission spectroscopy (ARPES) to
detect bulk Weyl points and surface Fermi arcs in TaAs and its cousins26–33 . ARPES is
an ideal tool for studying such a topological material, as known from the extensive body of
work on topological insulators4–6 . The ARPES technique involves shining light on a material
and measuring the energy, momentum, and spin of the emitted photoelectrons, both from
the surface and the bulk. This allows for the direct observation of both bulk Weyl points
and Fermi arc surface states. Weyl semimetals further give rise to fascinating phenomena in
transport, including a chiral anomaly in the presence of parallel electric and magnetic fields,
a novel anomalous Hall response, and exotic surface-state quantum oscillations. Even more
exotic effects may arise in the presence of superconductivity, where Weyl semimetals may
give rise to quasiparticles exhibiting non-Abelian statistics, potentially providing a platform
to realize novel effects in spintronics or a new type of topological qubit36–38 .
3
In this review, we survey the experimental discovery of the first Weyl semimetal in TaAs.
We first provide some key elements of the theory of Weyl semimetals. Then, we offer a
history and some intuition for Weyl semimetals from the point of view of a search problem.
Next, we review the key theoretical and experimental works of the discovery of the first
Weyl semimetal in TaAs by ARPES. We also discuss the discovery of Weyl semimetals in
the other compounds of the TaAs family, namely NbAs, TaP, and NbP. As an application
of the ARPES results, we discuss observation of the chiral anomaly in TaAs by transport.
We further mention briefly, but in no way attempt to discuss exhaustively, a wide range
of closely related topics, including: inversion-breaking Weyl semimetals beyond the TaAs
class, topological line node semimetals, strongly Lorentz violating Type II Weyl semimetals,
magnetic Weyl semimetals, and Weyl superconductors. These additional directions will no
doubt continue to enrich a fascinating and rapidly developing field of research.
The lattice constant is set to unity. Here, the σ are the Pauli matrices, k = (kx , ky , kz ) is
the crystal momentum, t is a hopping parameter and h(k) is the 2 × 2 Bloch Hamiltonian
±
matrix. We can see that at kW = (±k0 , 0, 0), all three of the functions a(k), b(k) and c(k)
±
simultaneously vanish. At these special kW the two bands are degenerate.
±
We can expand the Hamiltonian in the vicinity of the kW to derive a low-energy effective
± ±
model. We note that a(k) ≈ (k − kW ) · ∇a(kW ) and similar for b(k), c(k). We define
4
±
p± ≡ k − kW and we find that the low-energy model gives a cone-shaped dispersion,
h± (p) = vx p± ± ±
x σx + vy py σy + vz pz σz (2)
vx = −t sin(±k0 ), vy = vz = t
HW (p) = p · σ (3)
However, we note that unlike HW (p), our effective theory h± (p) shows a Weyl fermion
which has different Fermi velocities in different momentum directions, and so is not isotropic.
This behavior is quite reasonable because Lorentz invariance is not required in low-energy
effective theories in crystals. Next, we consider the effect of adding small, arbitrary perturba-
tions to h(k), taking a0 (k) = a(k) + ∆a(k) and similar for b(k), c(k). Will such perturbations
± ± ±
gap out the Weyl cones? To lowest order, we find a0 (k) ∼ (k − kW ) · ∇a0 (kW ) + ∆a(kW )=
± ±
(k − (kW + ∆k ± )) · ∇a0 (kW ), where ∆k ± in general will depend on all three of the perturbing
functions ∆a(k), ∆b(k) and ∆c(k). We see that the low-energy Hamiltonian remains gapless,
but that the Weyl points move around in momentum space as we perturb the system.
The local stability of the Weyl points is related to the Chern number, a topological
invariant well-known from the integer quantum Hall effect. The Chern number χ is defined
as,
ZZ
1
χ= dkx dky ẑ · Ω, Ω = ∇k × A, A = −ihk, n|∇k |k, ni (4)
2π
Here, A is the Berry connection and Ω is the Berry curvature. In the case of the integer
quantum Hall effect, the system is two-dimensional, so we integrate over the entire Brillouin
zone. To find the Hall conductivity of a quantum Hall state, we further sum the result over
all occupied bands n. In the case of a Weyl semimetal, the system is three-dimensional,
so we must choose some closed two-dimensional manifold within the bulk Brillouin zone
and calculate the Chern number on that manifold. If we choose a small spherical manifold
enclosing the Weyl point, we find that the Weyl point is associated with a Chern number
χ = ±1. We refer to this χ as the chiral charge of the Weyl point. The chiral charge
measures the Berry flux through the spherical manifold, analogous to Gauss’s law in classical
electrodynamics. In the same way as for an electric charge, the chiral charge is quantized
and the Chern number on any manifold depends only on the enclosed chiral charge.
5
It is clear that Weyl points arise generically in two-band models. In particular, the
underlying mathematics does not care about the basis of the Hamiltonian. Typically, a
Weyl semimetal refers to a normal electron system, but the basis can also be a Bogoliubov
spinor, describing a Weyl superconductor, or it may consist of bosonic particles, describing,
for instance, a photonic Weyl semimetal. At the same, it is important to note that most
normal electron crystals have both time reversal and inversion symmetry, which requires all
bands to be everywhere doubly-degenerate. In such a system, a band crossing corresponds
to a four-fold degeneracy, requiring a description by a four-band model. However, in a four-
band model, there are too many Hamiltonian matrix elements that must be simultaneously
set to zero, so band crossings do not arise generically. In this way, the experimental study
of Weyl semimetals has long been held back because nature prefers to maintain both time
reversal and inversion symmetries.
If Weyl points are topologically stable, we might ask how they can be created or de-
stroyed. While an individual Weyl point cannot be gapped out within band theory by small
perturbations, a large perturbation can cause Weyl points of opposite chirality to annihilate
each other, leaving the system gapped. If we imagine slowly applying a large perturbation
to h(k), we will find that the Weyl points move around in momentum space until the system
arrives at a critical point where the Weyl points sit on top of each other. A further pertur-
bation can then cause the system to gap out. Conversely, Weyl points can only be created
through such a critical point, in sets of equal and opposite chiral charge. An equivalent
statement is that the net chiral charge in the entire Brillouin zone is always zero. It is also
possible to gap a Weyl point by going beyond band theory. If h(k) is taken to describe a
normal electron system, then superconductivity may gap the Weyl points by breaking U (1)
charge conservation symmetry. A charge density wave or disorder may also allow scattering
±
directly between the kW , gapping the Weyl cones by breaking translation symmetry. In
this sense, Weyl points are protected by charge and translation symmetries. By contrast,
the Dirac points in graphene3 , topological insulators4,6 and Dirac semimetals29 typically re-
quire not only the symmetries implied within band theory, but further rely on time reversal
symmetry, inversion symmetry or other crystal space group symmetries. We see that Weyl
points are uniquely robust in that they are topologically stable within band theory without
any additional symmetries.
The integer quantum Hall effect is associated with gapless chiral edge modes guaranteed
6
by the Chern number. What boundary states are guaranteed by Chern numbers in Weyl
semimetals? We consider two-dimensional slices of the bulk Brillouin zone, as shown in
Fig. 1c-e. Any slice not containing the Weyl points is gapped, and we can calculate a Chern
number for that slice. In this way, we can view the three-dimensional band structure as a
set of two-dimensional slices with a tuning parameter, kx . As we scan kx , the bulk band gap
closes and reopens and we tune the system through a topological phase transition, changing
the Chern number. The critical slices kx = ±k0 are the slices containing a Weyl point. We
can similarly partition the surface states of a Weyl semimetal into one-dimensional edges,
as shown in the surface Brillouin zone square in Fig. 1d. Edges associated with a non-zero
Chern number in the bulk will host gapless chiral edge modes, Fig. 1e, while edges with a
zero Chern number are gapped, Fig. 1c. We can see that these one-dimensional edge states
then assemble into a sheet of surface states which terminate at the surface projections of the
Weyl points, forming a topological Fermi arc surface state. On a constant-energy cut of the
surface band structure, the Fermi arc forms an open, disjoint curve. Much like the Dirac
cone surface state of a three-dimensional Z2 topological insulator, the Fermi arc of a Weyl
semimetal is anomalous in the sense that it cannot arise in any isolated two-dimensional
system, but only on the two-dimensional boundary of a three-dimensional bulk. However,
the Fermi arc arguably provides the most dramatic example to date of an anomalous band
structure, because unlike the Dirac cone surface state or any traditional two-dimensional
band structure, the constant-energy contours do not even form closed curves.
The paramount experimental challenge to the discovery of the first Weyl semimetal was
finding suitable material candidates. It was necessary to find compounds available in high-
quality single crystals with Weyl fermions and Fermi arcs accessible under reasonable mea-
surement conditions. In the five years or so preceding the discovery of TaAs, roughly from
2011 to 2015, the fundamental theory of Weyl semimetals was essentially available and pow-
erful ARPES systems were ready to tackle the problem. The missing link was the lack of
material candidates. In this section, we discuss the particular insights relating to material
7
search that bridged theory to experiment and directly opened the experimental study of
Weyl semimetals. We also highlight some open problems along these directions.
It was perhaps a historical accident that the community initially focused on time-reversal
breaking Weyl semimetals. After Murakami’s work showing a connection between Weyl
semimetals and topological insulators16 , Wan et al. proposed in 2011 the first material can-
didate for a Weyl semimetal in a family of magnetic pyrochlore iridates, R2 Ir2 O7 , where R
is a rare-earth element17 . In this crystal, the Ir atoms form a sublattice of corner-sharing
tetrahedra and the authors argued that the material prefers an all-in/all-out configuration of
magnetic moments on the tetrahedra, breaking time-reversal symmetry17 . Next, theoretical
analysis showed that, by increasing the on-site Coulomb interaction strength, the system
exhibits a transition from a magnetic metal to a Mott insulator. In between, there is an
intermediate phase, which was found to be a Weyl semimetal. Wan et al. also made an
explicit connection between Weyl semimetals and the integer quantum Hall (IQH) state.
Specifically, they proposed the idea of calculating Chern numbers on two-dimensional mani-
folds in the three-dimensional Brillouin zone of a bulk material. In a Weyl semimetal, there
would be manifolds with nonzero Chern numbers. As in the IQH effect, the one-dimensional
edge of the two-dimensional manifold would protect chiral edge states and these would as-
semble together to form Fermi arc surface states on the two-dimensional surface of a Weyl
semimetal. The specific material proposal and theoretical advances spurred considerable
interest in Weyl semimetals. However, attempts to realize a Weyl semimetal in R2 Ir2 O7
in experiment were met with significant challenges. The all-in/all-out magnetic order is
under debate in experiments41,42 . Also, while metal-insulator transitions were observed in
Eu2 Ir2 O7 and Nd2 Ir2 O7 39,40 and transport and optical behaviors were roughly consistent with
a semimetal or a narrow band-gap semiconductor40,43 , the results overall were inconclusive.
At the same, ARPES measurements are lacking, possibly because it has been difficult to
grow large, high-quality single crystals or because it has been difficult to prepare a flat
sample surface for measurement.
Shortly following the proposal for a time-reversal breaking Weyl semimetal in R2 Ir2 O7 ,
Burkov and Balents proposed, also in 2011, an engineered time-reversal breaking Weyl
semimetal in a heterostructure built up from topological insulator and magnetic layers19 .
They provided a simple tight-binding model which explicitly includes the necessary ingredi-
ents for a Weyl semimetal and shows only two Weyl points, providing the “hydrogen atom”
8
of a Weyl semimetal in theory. They also point out that their model shows a non-quantized
anomalous Hall conductivity proportional to the separation of Weyl points in momentum
space. Despite its theoretical significance, this model has remained unrealized in experiment.
It requires a topological insulator and a trivial insulator with suitable lattice match that
can both be grown by a thin film technique such as molecular beam epitaxy. In addition,
magnetism must somehow be incorporated into the system, either by doping or perhaps by
replacing the trivial insulator with a ferromagnet. Studying the emergent band structure of
such a system in experiment would also be a formidable challenge.
Similar in spirit was a subsequent work by Bulmash et al., who in 2014 proposed engineer-
ing a time-reversal breaking Weyl semimetal by doping a topological insulator44 . Specifically,
they proposed starting with HgTe, a three-dimensional topological insulator, tuning it to
the critical point for a band inversion by Cd doping and then introducing a magnetic order
through Mn doping, giving Hg1−x−y Cdx Mny Te. Again, this proposal was quite reasonable
in that it introduced the key ingredients for a Weyl semimetal in an explicit way through
doping. Like the proposal by Burkov and Balents, the resulting system would also have only
two Weyl points. However, despite the conceptual elegance of this work, ARPES measure-
ments on Hg1−x−y Cdx Mny Te were unsuccessful. One reason might be that disorder from
doping degraded sample quality too severely.
With the arrival of topological Dirac semimetals in Na3 Bi and Cd3 As2 29,45–49 , the commu-
nity also considered magnetic doping of a Dirac semimetal as a way to realize a time-reversal
breaking Weyl semimetal, although there are no formal published proposals. These ideas
were close to the work by Bulmash et al., but now the Dirac semimetal state was achieved
intrinsically and only the time-reversal breaking needed to be implemented by doping. In-
deed, these proposals faced difficulties similar to the case of Hg1−x−y Cdx Mny Te. Specifically,
it was challenging to grow high-quality single crystals with magnetic doping which gave rise
to a useful magnetic order. Another concern is that the spin-splitting from a magnetic dop-
ing may be too small to produce Weyl points above available experimental resolution and
spectral linewidth in an ARPES measurement.
It was gradually appreciated that an intrinsic material may be easier to study than an
engineered or doped system. However, finding an intrinsic time-reversal breaking Weyl
semimetal presents its own challenges. The original proposal for R2 Ir2 O7 is a case in point,
because the magnetic order is difficult to predict from calculation and has not been conclu-
9
sively shown in experiment. Also, it is unclear whether the value of the correlation parameter
U appropriate for the real material actually places the system in the Weyl semimetal phase.
In 2011, the same year of the proposal for R2 Ir2 O7 and the topological insulator multilayer,
Xu et al. proposed a Weyl semimetal in HgCr2 Se4 21 . Unlike R2 Ir2 O7 , HgCr2 Se4 is known to
be an intrinsic ferromagnet with a Curie temperature, TC ' 120 K, which is easily accessible
in experiment. ARPES experiments on this system were not successful, perhaps because
crystals are not of sufficiently high quality. However, recently, evidence for half-metallicity
was reported in transport experiments, which may lead to renewed interest in this material50 .
Another interesting property is that the bands responsible for the band inversion arise from
Hg and Se, while the ferromagnetism is associated with Cr. This makes the band inversion
in ab initio calculation robust to changes in U . Nonetheless, one concern is that the cubic
structure of HgCr2 Se4 allows many magnetization axes, which may favor the formation of
small magnetic domains. It remains a considerable experimental challenge to create large
magnetic domains in situ, as well as to understand whether a Weyl semimetal could be
shown in an ARPES experiment which averages over many magnetic domains. Nonetheless,
the proposal for HgCr2 Se4 offers an approach to searching for new candidates. In particular,
it may be fruitful to study systems with an experimentally well-known magnetic order and
where the Weyl semimetal state is robust to free parameters in the ab initio calculation.
As the experimental complications of time-reversal breaking Weyl semimetals were ap-
preciated, it was understood that breaking inversion symmetry may provide an easier route
to the first Weyl semimetal. In retrospect, this should be rather clear. While the effect
of breaking inversion symmetry and time-reversal symmetry is mathematically similar at
the level of a single-particle Hamiltonian, these two symmetries relate to deeply different
phenomena in any real material. Inversion symmetry breaking is a property of a crystal
structure, which can be measured directly by X-ray diffraction and presents no particular
complications to ab initio calculation. By contrast, magnetism is a correlated phenomenon
which is extremely difficult to reliably predict from first principles, challenging to under-
stand in experiment and difficult to accurately capture in an ab initio calculation even if
the magnetic order is experimentally known. Additional complications arise because exper-
iments must be carried out below the magnetic transition temperature and a measurement
may average over many small magnetic domains. By contrast, large inversion breaking do-
mains have been observed in inversion breaking materials. A well known example is the bulk
10
Rashba material BiTeI, where the bulk Rashba splitting due to inversion breaking can be
directly observed in ARPES. The idea that inversion breaking systems are simpler reignited
the search for Weyl semimetals and led to the prediction and experimental observation of
the first Weyl semimetal in TaAs.
Before discussing the theoretical prediction of TaAs, we note that despite the early focus
on time-reversal breaking Weyl semimetals, there was some interest in inversion breaking
systems. In 2012, Singh et al. considered the tunable topological insulators TlBi(S1−x Sex )2
and TlBi(S1−x Tex )2 and proposed to engineer a Weyl semimetal by alternating between Se
and Te from layer to layer, which would break inversion symmetry22 . While this proposal
was directly motivated by the recent experimental success in realizing a topological phase
transition in TlBi(S1−x Sex )2 22,23,29 , the expected separation of the Weyl points in the pro-
posed system fell below available experimental resolution in ARPES. Halász and Balents
proposed in 2012 an inversion-breaking Weyl semimetal in a HgTe/CdTe heterostructure,
inspired by a superlattice model similar to the time-reversal breaking model in a topological
insulator multilayer51 . This proposal remains unrealized, perhaps for reasons similar to the
earlier proposal by Burkov and Balents, that there are considerable experimental challenges
to studying the emergent band structure of such a superlattice. Lastly, in 2014, Liu and
Vanderbilt proposed realizing an inversion breaking Weyl semimetal by tuning an inversion
breaking topological insulator through a topological phase transition, exactly as first dis-
cussed by Murakami52 . Specifically, they predict a Weyl semimetal in LaBi1−x Sbx Te3 and
LuBi1−x Sbx Te3 for x ∼ 38.5% − 41.9% and x ∼ 40.5% − 45.1%. This proposal also remains
unrealized, perhaps because the calculation results suggest that the Weyl semimetal phase
is extremely sensitive to the composition x. Nonetheless, such tunable inversion breaking
systems are of considerable interest because they would exhibit a topological phase tran-
sition to a Weyl semimetal, which to date is unrealized. Realizing such a system may
require us to understand why the Weyl semimetal phase is so narrow in LaBi1−x Sbx Te3 and
LuBi1−x Sbx Te3 and whether this behavior is natural.
The material search for intrinsic inversion breaking Weyl semimetals was based on a broad
foundation of known crystal structures. These have been accumulated by X-ray diffraction
experiments performed over the course of a century or more of research in physics and
chemistry and which have been cataloged in databases such as the Inorganic Crystal Struc-
ture Database of FIZ Karlsruhe. Certain catalogs of magnetic compounds also exist with
11
measurements of magnetic transition temperatures or magnetic structures. These sources
provided a starting point for material searches. It is worth noting that nature prefers to
maintain both inversion and time-reversal symmetry, severely limiting from the outset the
number of possible material candidates for both kinds of Weyl semimetals.
Although ab initio calculations for inversion-breaking systems are simpler, the calculation
is still challenging because Weyl points typically occur at arbitrary k points rather than at
high symmetry points or on high symmetry lines. As a result, for each compound, it is
necessary to calculate the band structure at all k points throughout the bulk Brillouin zone
to demonstrate or exclude the existence of Weyl points. A large spin-orbit coupling is
preferred to produce a large spin-splitting. A closely-related requirement is that the Weyl
points should be well-separated. Materials which also crystallize in an inversion-symmetric
structure are excluded. The Weyl points should be very near the Fermi level and, for
future transport experiments, it is preferable to find systems without irrelevant pockets
at the Fermi level. The materials conditions such as cleavability and large single domain
crystallinity that make ARPES measurements feasible were also considered to narrow down
the candidate list further. In 2014, TaAs emerged as a promising candidate satisfying
these ARPES criteria26,27 . Shortly thereafter, in early 2015, the observation of bulk Weyl
fermions and topological Fermi arcs were finally reported in TaAs, demonstrating the first
Weyl fermion semimetal28,32 .
With the recipe for an inversion-breaking Weyl semimetal better understood, many other
inversion-breaking Weyl semimetals were proposed55–64 . Here, we do not attempt to survey
these later inversion-breaking Weyl semimetal candidates. These systems will no doubt lead
to many fascinating directions of research in the future.
12
in bulk TaAs single crystals, demonstrating a Weyl semimetal at the same time in the bulk
and on the surface and in excellent agreement with calculation.28 . Equivalently, a nonzero
Chern number was directly measured from the Fermi arcs. These observations confirmed
the bulk-boundary correspondence between Weyl cones and topological Fermi arcs. The
discovery of the first Weyl semimetal in TaAs not only opened a new chapter in the study of
topological phases of matter, but also validated the shift of the community from time-reversal
breaking candidates to inversion breaking candidates. The identification of TaAs was quickly
followed by the discovery of Weyl semimetals in NbAs30 and TaP31,73 , with additional work
on NbP35,74–76 . Below, we review the experimental discovery of Weyl semimetals by ARPES
in TaAs and its cousins. We also discuss general criteria for demonstrating a Weyl semimetal
in ARPES, which arose from studies of these compounds35 .
13
correspond to the projected Weyl points with projected chiral charge ±2.
Both Weyl cones and Fermi arcs were observed by ARPES, each of which independently
demonstrate the Weyl semimetal state in TaAs28,32,33 . The Weyl points and Weyl cones
in TaAs were accessed by ARPES measurements at soft X-ray photon energies, which are
sensitive to the bulk states. Soft X-ray data showed that the Fermi surface of TaAs consists
of discrete points at specific incident photon energies and binding energies, at generic points
in the Brillouin zone (Fig. 3a). Away from these discrete points in binding energy, the
bands dispersed linearly in both the in-plane momenta, kx and ky (Figs. 3b,c) and the out-
of-plane momentum kz (Figs. 3d). The observation of linearly-dispersing band crossings at
generic points in the bulk Brillouin zone demonstrated Weyl points and Weyl nodes in TaAs,
showing that TaAs is a Weyl semimetal.
Independently of the bulk-sensitive soft X-ray ARPES measurements, surface-sensitive
ARPES measurements at vacuum ultraviolet photon energies showed Fermi arcs on the (001)
surface of TaAs. The ARPES measured Fermi surface showed three dominant features: a
bowtie-shaped feature centered at the X̄ point, a elliptical feature centered at the Ȳ point,
and a crescent-shaped feature near the midpoint of each Γ̄− X̄(Ȳ ) line (Fig. 4a). The results
were in excellent agreement with the ab initio calculation (Fig. 2e). More extensive APRES
measurements of the crescent showed that it consists of two segments joined together at their
endpoints (Fig. 4b), strongly suggesting Fermi arcs. Ab initio calculation showed topological
Fermi arcs in close agreement with the crescent observed in ARPES, showing that Fermi
arcs were observed. A non-zero Chern number was also directly observed, providing another
demonstrating of Fermi arcs from the ARPES data, see discussion below. Finally, ARPES
data also showed that the terminations of the Fermi arcs coincide with the projections of
the Weyl nodes, which demonstrated the bulk-boundary correspondence principle (Fig. 4d),
further confirming the observation of a Weyl semimetal in TaAs28 . Later measurements by
spin-resolved ARPES showed the spin texture of the Fermi arcs77,78 . In calculation, the spin
texture was found to wind against the dispersion of the Fermi arc, so that if we traverse the
Fermi arc in a clockwise way, the spin texture winds in a counter-clockwise way (Fig. 4c).
This spin texture was directly measured by spin-resolved ARPES and was found to be in
excellent agreement with the ab initio calculation (Fig. 4e,f ). The relationship of the spin
texture to the topological invariants of the bulk is not understood. It appears that there is
no obvious constraint placed on the Fermi arc spin texture by the chiral charge of the Weyl
14
points. We note that no spin-resolved soft X-ray ARPES end-station is currently available,
which has hindered the measurement of the spin texture of the Weyl points and Weyl cones.
This has prevented the direct experimental measurement of the chiral charge in a Weyl
semimetal. To directly measure the chiral charge, either the appropriate ARPES system
must become available or a new material is needed where the bulk band structure can be
accessed by vacuum ultraviolet ARPES.
A non-zero Chern number in TaAs was directly measured from an ARPES spectrum
of the surface states35 . The authors considered a cylindrical tube in the bulk Brillouin
zone enclosing two Weyl points of the same chiral charge. The Chern number on this two
dimensional manifold is +2 (Fig. 5a). As a result, the one-dimensional edge of the cylindrical
slice hosts protected chiral edge states which cross the bulk band gap and have net chirality
+2 (Fig. 5b). In this way, a Chern number can be directly measured in an ARPES spectrum
of the surface state band structure by counting the net chirality of surface state crossings on a
closed loop in momentum space (Fig. 5c). It was found in ARPES that the one-dimensional
band structure on the loop showed two edge states of the same chirality at the Fermi level,
in agreement with the topological theory (Fig. 5d). The direct measurement of a non-zero
Chern number in TaAs by ARPES provides yet another independent demonstration that
TaAs is a Weyl semimetal.
The case of TaAs showed that topological Fermi arcs do not always appear as disjoint
arcs. Specifically, in TaAs, the Fermi arcs appeared in pairs which together formed a closed
contour. As a result, the signature of a Fermi arc in the experiments on TaAs was not a
disjoint arc but rather a Chern number or a surface state kink, as discussed above. More
generally, it was directly relevant for experiment to understand the ways that a topological
Fermi arc can arise in a material. As far as is currently understood, there are four distinct
criteria for topological Fermi arcs35 . All signatures are in principle experimentally accessible
in an ARPES measurement of a surface state band structure. Each signature alone, observed
in any set of surface state bands, is sufficient to show that a material is a Weyl semimetal,
1. Disjoint arc: Any surface state constant-energy contour with an open curve is a Fermi
arc and demonstrates a Weyl semimetal.
15
2. Kink off a rotation axis: A Weyl point is characterized by chiral charge n, equal to
the Chern number on a small spherical manifold enclosing the Weyl point in the bulk
Brillouin zone, illustrated by the small sphere in Fig. 5(e)8,17,65 . For a Weyl point of
chiral charge |n| > 1 or if multiple Weyl points project onto the same point of the
surface Brillouin zone, there may not be a disjoint constant-energy contour because
multiple arcs will emanate from the same Weyl point projection. However, the arcs
will generically attach to the Weyl point at different slopes, giving rise to a kink in the
constant-energy contour. Moreover, such a kink can only arise from the attachment of
two Fermi arcs. A kink on the projection of a rotation axis may arise in a topological
Dirac semimetal29 . Off a rotation axis, such a kink guarantees a Weyl semimetal.
3. Odd number of curves: For projected chiral charge |n| > 1, the constant-energy con-
tours may consist entirely of closed curves and the kink may be below experimental
resolution, so the constant-energy contour appears everywhere smooth. However, if
|n| is odd, the constant-energy contour will consist of an odd number of curves, so at
least one curve must be a Fermi arc.
4. Non-zero Chern number : Consider any closed loop in the surface Brillouin zone where
the bulk band structure is everywhere gapped and, at some energy, add up the signs
of the Fermi velocities of all surface states along this curve, with +1 for right movers
and −1 for left movers. The sum is the projected chiral charge enclosed in the curve,
corresponding to a Chern number on a bulk8,17,65 . A non-zero sum on at least one
loop demonstrates a Weyl semimetal, provided the loop is chosen to be contractible
on the torus formed by the surface Brillouin zone.
Note that while (1), (2) and (3) describe properties of a constant-energy slice of the Fermi
surface, the counting argument (4) requires a measurement of the dispersion. We note also
that criterion (4) allows us to determine all bulk topological invariants and Weyl points of
a material by studying only its surface states.
One caveat in this rather formal analysis is that in a real ARPES experiment we never
rigorously measure only the surface or bulk states, but rather some combination of the two.
There are, furthermore, many experimental scenarios where a surface state unrelated to
Fermi arcs can naı̈vely satisfy one of the criteria. For instance, the photoemission cross
section of certain bands or certain regions of a band may be suppressed under particular
16
measurement conditions. This effect can give rise to an apparently disjoint contour or an
apparent Chern number in a completely topologically trivial material. In addition, a kink
will always be smeared out in an experiment, so that it can be challenging to distinguish
between a kink and a smooth but rapidly dispersing band. Therefore, an ab initio calcula-
tion remains crucial for ARPES studies of new Weyl semimetal candidates. However, it is
equally unacceptable to simply show a general agreement between an ARPES spectrum and
a calculation. We note that a number of early works claimed to show a Weyl semimetal by
ARPES in TaAs and NbP by measuring a Chern number, but those measurements depended
on resolving Fermi arcs which clearly fell below any available experimental resolution or spec-
tral linewidth32,72,74–76 . As a result, those works essentially used a rough, overall agreement
between calculation and experiment to claim a Weyl semimetal. A reasonable standard for
detection of a Weyl semimetal in ARPES is to consider a set of surface states which can be
confirmed in calculation to be topological Fermi arcs and which can be clearly identified in
an ARPES spectrum. These Fermi arcs will not always show up as disjoint arcs, but they
must satisfy at least one of the four criteria discussed here.
It is known in quantum field theory that quantum fluctuations can violate classical conser-
vation laws, a phenomenon called a quantum anomaly79 . Perhaps the best-studied example
is the chiral anomaly associated with Weyl fermions15,80,81 . Historically, the chiral anomaly
was crucial in understanding a number of important aspects of the Standard Model of par-
ticle physics, such as the triangle anomaly associated with the decay of the neutral pion
π 0 , Refs.80,81 . Despite having been discovered more than 40 years ago, quantum anomalies
remained solely in the realm of high-energy physics.
The discovery of Weyl fermion semimetals provides a natural route to realizing the chiral
anomaly in condensed matter physics. Consider a Weyl semimetal with a particular con-
figuration of Weyl points of positive and negative chiral charge in the bulk Brillouin zone.
Parallel magnetic and electric fields can pump electrons between Weyl cones of opposite
chirality, giving rise to a population imbalance between Weyl cones of positive and nega-
tive chiral charge. This means that the numbers of Weyl fermions of a given chirality are
not separately conserved15,82–85 . The key observable consequence of the chiral anomaly in
17
a condensed matter system is that the longitudinal resistance is predicted to decrease as a
function of an external magnetic field, giving rise to a negative longitudinal magnetoresis-
tance (LMR). Except for this natural platform, Dirac semimetals, a class of materials that
host Dirac fermion quasiparticles, may similarly give rise to a negative LMR under external
magnetic field. In that case, the magnetic field not only directly produces a chiral anomaly
but additionally serves the purpose of splitting the Dirac cone into a pair of Weyl cones of
opposite chirality by breaking time-reversal symmetry. It is worth noting that under such
conditions, extra caution is needed, because in real materials a magnetic field may have
many effects other than a simple Zeeman splitting of the band structure107 .
The negative LMR was directly detected in electrical transport experiments on the TaAs
family96–105 (Figs. 6a-c) and a number of Dirac semimetals86–88 . Other supporting evidence
includes: (1) The negative LMR was prominent only in the geometry of parallel electric
~ ·B
and magnetic fields. This is consistent with the E ~ term in the chiral anomaly formu-
lation (Fig. 6c). (2) The negative LMR did not depend on the electrical current direction
with respect to the crystalline axis (Figs. 6a,b). However, these data are not conclusive.
A number of other effects can also lead to a negative LMR in metals89–95 , and some of
them92,95 may show the same systematic dependences as described above. Hence, to achieve
an unambiguous proof, further study is needed. One particular phenomenon that may pro-
vide stronger evidence is the dependence of the LMR on chemical potential. Because Weyl
points are monopoles of Berry curvature, the magnitude of negative LMR is expected to
follow a dramatic 1/EF2 dependence as the Fermi level moves away from the energy of the
Weyl points. This EF dependence97 (Fig. 6d) can distinguish the chiral anomaly from other
negative LMR effects and, therefore, provides a clearer demonstration of the chiral anomaly
due to Weyl fermions.
V. OUTLOOK
It has been less than a year since the experimental realization of the first Weyl semimet-
als, and the field has already evolved dramatically. One topic of recent interest is the
realization in a material of a strongly Lorentz-violating Weyl fermion. Traditionally, stud-
ies of Weyl fermions in quantum field theory were concerned with applications to particle
18
physics, where Lorentz symmetry is respected. However, low-energy effective field theories
in crystals need not satisfy Lorentz invariance, providing a richer variety of allowed theories.
In particular, the form of the dispersion of a Weyl fermion in a crystal has more freedom
than in particle physics. Recently, it was pointed out that this freedom allows for a novel
type of Weyl fermion where the Weyl cone is tipped over on its side58,66–68 . Such strongly
Lorentz-violating, or Type II, Weyl fermions allow us to study, in table-top experiments,
exotic Lorentz-violating theories that are beyond the Standard Model. They also open up
experimental opportunities for studying novel spectroscopic and transport phenomena spe-
cific to Type II Weyl fermions. Such phenomena include a chiral anomaly associated with a
transport response that depends strongly on the direction of the electric field, an antichiral
effect of the chiral Landau level, a modified anomalous Hall effect, and emergent Lorentz
invariance arising from electronelectron interactions58,66–71 . To date, Type II Weyl fermions
have only been suggested in W1−x Mox Te2 58–60 and observed in LaAlGe56,57 . Therefore, it is
of importance to continue the study of Type II Weyl semimetals.
Because the TaAs family exhibits twelve pairs of Weyl points, it is of some interest to
find simpler materials with fewer Weyl points. Material searches are under way to find the
“hydrogen atom” versions of Weyl semimetals with the minimum number of Weyl points
possible, either four Weyl points in inversion-breaking Weyl semimetals or two Weyl points
in magnetic Weyl semimetals. An additional challenge is to tune the materials so that
the Fermi level is close to the Weyl points, ideally within 5-10 meV, without irrelevant
pockets near the Fermi level, so that the Weyl fermionic excitations constitute the dominant
transport channel. Moreover, the T -breaking Weyl semimetals and Weyl superconductors
(both T -breaking and I-breaking) can give rise to a wide range of novel properties. To
understand the interplay between the electronic interaction and the topological state in
Weyl fermion semimetals, T -breaking magnetic Weyl materials could be crucial because
magnets already harbor strong interactions. From a purely mathematical point of view,
interacting Weyl phases further broaden the classification of topological phases of matter.
Exploring the nontrivial spin polarization properties of interacting Weyl materials could
reveal a rich phase diagram. In a loose sense, the spin texture is approximately proportional
to the Berry flux and, hence, projects like monopoles or antimonopoles near the Weyl nodes
in momentum space. This opens up opportunities for applications in spintronics. Realizing
Weyl superconductors would be another exciting frontier. The Majorana surface states of
19
a Weyl superconductor can be potentially used for topological qubits. Given the rapid
development of the field, it is also quite possible that in a few years, the most exciting
frontier will be something not projected here.
VI. ACKNOWLEDGMENTS
The authors thank Adam Kaminski, Arun Bansil, BaoKai Wang, Bingbing Tong, Cheng
Guo, Chenglong Zhang, Chi-Cheng Lee, Chi Zhang, Chuang-Han Hsu, Daixiang Mou, Daniel
S. Sanchez, Donghui Lu, Fangcheng Chou, Fumio Komori, Guang Bian, Guoqing Chang,
Hai-Zhou Lu, Hao Zheng, Hong Lu, Horng-Tay Jeng, Hsin Lin, J. D. Denlinger, Jie Ma,
Junfeng Wang, Kenta Kuroda, Koichiro Yaji, Lunan Huang, Madhab Neupane, Makoto
Hashimoto, Mykhailo L. Prokopovych, Nan Yao, Nasser Alidoust, Pavel P. Shibayev, Raman
Sankar, Shik Shin, Shuang Jia, Shun-Qing Shen, Sungkwan Mo, Takeshi Kondo, Tay-Rong
Chang, Titus Neupert, Vladimir N. Strocov, Xiao Zhang, Yun Wu, Zhujun Yuan and Ziquan
Lin for collaborations. Work at Princeton University by S.-Y.X. and M.Z.H. is supported
by the US Department of Energy under Basic Energy Sciences Grant No. DOE/BES DE-
FG-02-05ER46200 and Grant No. DE-AC02-05CH11231 at the Advanced Light Source at
Lawrence Berkeley National Laboratory (LBNL), and Princeton University funds. M.Z.H.
acknowledges Visiting Scientist user support from LBNL and partial support from the Gor-
don and Betty Moore Foundation under Grant No. GBMF4547/Hasan. Shin-Ming Huang
acknowledges visiting scientist support from Princeton University.
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27
a b
ࢿ ࢿ
Breaking
or
symmetry
Fermi arc
28
FIG. 1: Weyl fermions on a lattice. a, One way to create a Weyl semimetal is to start with
a massless Dirac fermion in a system with both time reversal and inversion symmetries. Such a
Dirac fermion corresponds to the intersection of two doubly-degenerate bands and can be realized,
for instance, at the critical point of a topological phase transition between a normal insulator and
a topological insulator. b, By breaking time reversal or inversion symmetry, the Dirac fermion
splits into a pair of Weyl fermions of opposite chiralities. Each Weyl fermion is a monopole or
anti-monopole of Berry curvature and, equivalently, is associated with a Chern number. The
Chern number guarantees the existence of a topological Fermi arc surface state that connects the
projections of the Weyl points in the surface Brillouin zone. c-e, Weyl semimetals are characterized
by Chern numbers, as in the integer quantum Hall effect. For instance, we can consider a system
with two Weyl points of chirality ±1 and we can calculate the Chern number on slices of the
Brillouin zone at different kx , d. When a slice is swept through a Weyl point, the two-dimensional
system undergoes a topological phase transition and the Chern number changes by ±1. For slices
with a Chern number ν = 0, the one-dimensional edge of the two-dimensional slice is gapped, c,
while slices with a Chern number ν = +1 host a protected gapless chiral edge mode, e. The Fermi
arc can be understood as arising from all of the chiral edge states assembled together into a surface
state.
29
a b c 2
-2
-4
-6
1 nm
As(P) -8
Ta(Nb) Γ Σ N Σ1 Z Γ X
d e
W2
1 Γ
W1
kz (2π/c)
0
0.5
0
-0.5
0 ky (2π/a)
0.5 -0.5
kx (2π/a)
FIG. 2: The crystal and electronic structures of the Weyl semimetal TaAs. a, Body-
centered tetragonal structure of TaAs. The crystal lattice lacks an inversion center. b, Scanning
tunneling microscopy (STM) topographic image of the (001) surface of TaAs, revealing a square
lattice. c, Survey of the band structure of TaAs. At this level, the system is quite simple, with
only two bands, a conduction and valence band, in the vicinity of the Fermi level, which approach
each other on the Σ − N − Σ1 line. d, The conduction and valence bands cross each other, forming
nodal crossing points in k-space where the bulk energy gap vanishes. This panel shows the nodal
crossing points in the bulk Brillouin zone. In the absence of spin-orbit coupling, the nodal crossing
points are nodal-lines, i.e. 1D rings, on the kx = 0 mirror plane, Mx , and two nodal-lines on the
ky = 0 mirror plane, My . In the presence of spin-orbit coupling, each nodal-line vaporizes into
six 0D nodal points, the Weyl nodes. The Weyl nodes are denoted by small circles. Black and
white show the opposite chiral charges of the Weyl points. We denote the 8 Weyl nodes located on
the kz = 2π/c plane as W1 and the other 16 nodes away from this plane as W2 . e, Theoretically
calculated (001) surface-state Fermi surface. Adapted with modifications from Ref.28 .
30
a 1
b
0
High
/ 0.5
eV
1
-0.5
Low
-1
2
-1 -0.5 0 0.5 1 -0.5 0 0.5
/ || /
c d
0
0 Weyl Weyl
eV
eV
0.4
0.2
0.4 0.8
-0.2 0 0.2 50 51 52 53 54
|| /
31
a b c
1.5 -0.2
ky (Å-1)
ky
-0.4
1.0
M
-0.6
0.5 -0.1 0.0 0.1 kx
ky (Å-1)
Y kx (Å-1)
0.0
d
Γ
-0.5
kz
-1.0 X
ky
0.0 0.5 1.0 kx
kx (Å-1)
e f 0.8
0.8
0.4
Spin polarization
Spin polarization
0.4
0.0 0.0
-0.4 -0.4
-0.8 -0.8
0.4 0.2 0.0 0.4 0.2 0.0
EB (eV) EB (eV)
32
FIG. 4: Topological Fermi arcs in TaAs. a, ARPES spectrum of the surface state band
structure of TaAs near the Fermi level, EF . The green dotted lines denote the boundaries of the
surface Brillouin zone. b, High resolution ARPES Fermi surface of the double Fermi arcs that
arise from a pair of projected W2 Weyl nodes. The k-space region of this map is indicated by the
blue box in panel (a). c, Theoretically calculated Fermi surface of the double Fermi arcs that arise
from the same pair of projected W2 Weyl nodes. We indicate schematically the spin texture of the
Fermi arcs. d, Lower box: illustration of four W2 Weyl nodes in the bulk Brillouin zone, two of
each chirality. Upon projection on the (001) surface Brillouin zone, the two +1 and the two −1
Weyl nodes project onto each other, giving a projected chiral charge of ±2. Top surface: ARPES
spectrum of the two Fermi arcs connecting the projected Weyl nodes. The black and white circles
in panels (b-d) show the projected W2 Weyl nodes with opposite chiralities. e,f, Spin polarization
along the kx direction, as measured in spin-resolved ARPES at two points on the Fermi arcs, as
indicated by the red and orange dots in (c). Adapted with modifications from Refs.28,78 .
33
Chern number = 2
a b
kloop
CB
EB
ky
kz
VB
kx kloop
c d
1.5
0.4
Chiral edge states
1.0 M
0.0
EB (eV)
0.5
ky (Å-1)
Y
0.0 -0.4
Γ
-0.5
-0.8
-1.0 X
0.0 0.5 1.0 0.0 0.4 0.8 1.2
kx (Å-1) kloop (Å-1)
e
34
FIG. 5: Bulk-boundary correspondence in the Weyl semimetal TaAs. a, Illustration of a
Chern number in TaAs. The blue and red dots are Weyl points of opposite chiralities. We consider
a cylindrical tube extending through the bulk Brillouin zone and enclosing two Weyl points of the
same chirality. There is a net enclosed chiral charge of +2, so the Chern number on this two-
dimensional slice of the Brillouin zone is +2. b, On the one-dimensional boundary of the tube, the
Chern number protects two chiral edge states, which make up one slice of the topological Fermi
arcs. c, We can directly demonstrate that TaAs is a Weyl semimetal from the surface state band
structure as measured in ARPES by drawing a loop in the surface Brillouin zone and counting
the crossings to show a nonzero Chern number. The loop is shown by the dotted black line. d,
The surface states along the loop. We find two edge states of the same chirality, showing a Chern
number of +2. Note that for a conventional electron or hole pocket, such a counting argument
will always give 0. (e) The four criteria for a topological Fermi arc. (1) A disjoint contour. (2) A
closed contour with a kink. (3) No kinks within experimental resolution, but an odd set of closed
contours. (4) An even number of contours without kinks, but net non-zero chiral edge modes.
Adapted with modifications from Refs.28,35 .
35
a b
c d e
the zero-field resistivity, ∆ρ = ρ(B) − ρ(B = 0), or the magnetoconductivity as determined from
∆ρ. d, Dependence of the chiral coefficient CW , appropriately normalized by the other fitting
coefficients, on chemical potential, EF . Remarkably, the observed scaling behavior is 1/EF2 , as
expected from the dependence of the Berry curvature on chemical potential in the simplest model
of a Weyl semimetal, Ω ∝ 1/EF2 . e, A cartoon illustrating the chiral anomaly in TaAs97 . The chiral
~ ·B
anomaly leads to an axial charge pumping, for E ~ 6= 0. This causes a population imbalance
between Weyl cones of opposite chiralities. The charge pumping reaches an equilibrium with the
axial charge relaxation, characterized by a timescale τa , Refs.84,85 . Note that the axial charge
relaxation time τa can be directly obtained from the observed negative LMR data through the
chiral coefficient CW = e4 τa /4π 4 ~4 g(EF ), as discussed elsewhere97 . Adapted with modifications
from Ref.97,106 .
36