Abstract
The phase offset of quantum oscillations is commonly used to experimentally diagnose topologically nontrivial Fermi surfaces. This methodology, however, is inconclusive for spinorbitcoupled metals where πphaseshifts can also arise from nontopological origins. Here, we show that the linear dispersion in topological metals leads to a T^{2}temperature correction to the oscillation frequency that is absent for parabolic dispersions. We confirm this effect experimentally in the Dirac semimetal Cd_{3}As_{2} and the multiband Dirac metal LaRhIn_{5}. Both materials match a tuningparameterfree theoretical prediction, emphasizing their unified origin. For topologically trivial Bi_{2}O_{2}Se, no frequency shift associated to linear bands is observed as expected. However, the πphase shift in Bi_{2}O_{2}Se would lead to a false positive in a Landaufan plot analysis. Our frequencyfocused methodology does not require any input from abinitio calculations, and hence is promising for identifying correlated topological materials.
Introduction
The discovery of topological semimetals promises an avenue to study novel materials that host quasiparticles that mimick relativistic Dirac and Weyl fermions in highenergy physics^{1,2,3,4}. They host bands that touch at points or lines in momentum space; such degeneracies are typically associated with closed Fermi surfaces with topologically robust Berry phases. While initially considered a rare occurrence, recent abinitio programs^{4,5,6,7} have predicted topological band degeneracies in a sixth of all nonmagnetic materials in the crystal database^{5}.
Magnetic quantum oscillations^{8} promise to play a key role in experimentally confirming these predictions. It is widely believed that a πphase shift in quantum oscillations is interpretable as a π Berry phase, and therefore a smokinggun confirmation of a topological semimetal. Such phase analysis, often carried out with a ‘Landaufan plot’, ignores other nongeometric phase shifts, and forgets that the Berry phase is not quantized to an integer multiple of π for many symmetry classes of (semi)metals^{9,10}. For this reason, an unambiguous topological diagnosis is generally impossible for the 3D Dirac semimetals^{1,2,3} and lowsymmetry 3D Weyl semimetals^{9}.
For these cases, we present a new identification method based on the temperature (T) dependence of the oscillation frequency (F), finding a characteristic T^{2} contribution that is uniquely attributed to the linear energymomentum dispersion of Dirac, Weyl and multifold fermions^{11}. This T^{2} contribution is a 3D, higherdegeneracy generalization of an effect predicted by Kübbersbusch and Fritz^{12} for 2D Dirac materials. To the best of our knowledge, this effect has never been experimentally studied in graphene, yet we will show that it is easy to see in 3D Weyl/Dirac materials. Our strategy applies to candidate topological Fermi pockets which are small compared to the Brillouinzone volume; small pockets are accurately described by k ⋅ p Hamiltonians that retain only the leadingorder term—giving a parabolic dispersion for the Schrödingertype fermion, and a linear dispersion for the Diractype fermion. These two cases are distinguishable by the energy derivative of the cyclotron mass m_{c} (Fig. 1). While ∂m_{c}/∂E = 0 for a parabolic dispersion, for a linear dispersion \(E(k)=\pm \sqrt{{({v}_{x}\hslash {k}_{x})}^{2}+{({v}_{y}\hslash {k}_{y})}^{2}}\), the particular energy dependence of the Fermisurface area S yields a nonzero energy derivative of the cyclotron mass:
with E_{F} the Fermi energy measured from the Dirac point and v_{j} the Fermi velocity.
To experimentally determine ∂m_{c}/∂E, we exploit the fact that quantum oscillations probe the band structure over an energy window (~k_{B}T) around the Fermi level, due to the thermal broadening of the FermiDirac distribution function. As lightermass particles experience less thermal damping than heavier particles, the effective frequency renormalizes towards lighter orbits as T increases. This effect is absent for parabolic bands because the effective mass is energyindependent. However, for a Diractype Fermi surface, the frequency decreases with increasing T because the effective mass is smaller closer to the node, as illustrated in Fig. 1a. This temperaturerenormalization of F applies generally to linear dispersions near band degeneracies, including Dirac and Weyl degeneracies, as well as higherfold degeneracies associated with Fermi pockets with higher Chern numbers (socalled ‘multifold fermions’)^{11}.
Results
General methodology
To quantify this frequency shift, it is useful to view the Lifshitz–Kosevich formula^{13,14} as an asymptotic expansion in powers of k_{B}T/E_{F} (the degeneracy parameter of Fermi gases). Odd powers of T modify the oscillation amplitude, with the first odd power giving the wellknown thermal damping factor; in contrast, even powers of T modify the frequency and phase. At elevated temperatures where 2π^{2}k_{B}T is large or comparable to the cyclotron energy, we derive in supplementary note 2(A) a T^{2}correction to the oscillation frequency:
with μ the chemical potential and β ≔ eℏ/2m_{c} the effective Bohr magneton. The correction ΔF^{top} is our main theoretical result, and applies to any closed Fermi surface originating from an arbitrary energymomentum dispersion, whether linear, quadratic, cubic or beyond. While ΔF^{top} vanishes for parabolic bands, it is finite for linear bands as \( \partial ({{{{{{\mathrm{log}}}}}}}\,{m}_{c})/\partial E =1/ {E}_{F}\), according to Eq. (1), and we hence refer to ΔF^{top} as a topological correction to F.
Next we consider other mechanisms for the temperature dependence of the frequency. A distinct T^{2} correction arises from the temperature dependence of the chemical potential [μ(T)] at fixed particle density, as is well known in the Sommerfeld theory of metals^{15} (Fig. 1b). The sum of Sommerfeld and topological corrections is expressed in:
with Θ a dimensionless coefficient. In highcarrierdensity metals with both small and large pockets, the Sommerfeld correction is negligible. The frequency shift of a small pocket is reduced by a factor ∣E_{F}∣/E_{bw} ≪ 1, with E_{F} the Fermi energy of the small pocket measured from band extremum/degeneracy, and E_{bw} the typical bandwith. Thus we expect that Θ is dominated by the topological correction, giving Θ ≈ 0 in the parabolic case, and Θ ≈ 1/16 in the case of a linear dispersion. For singlefrequency, lowcarrierdensity semimetals, the Sommerfeld correction is of the same order of magnitude as the topological correction, giving Θ = 1/48 for parabolic bands and Θ = 5/48 for linear bands [see supplementary note 2(B) for extended calculation of Sommerfeld correction]. The two scenarios show that the observation of a T^{2} correction alone is not conclusive of nontrivial topology. Rather, conclusiveness comes from the following experimental consistency check: since F_{0}(E_{F}), m_{c} and additionally the frequency shift at elevated temperatures all can be experimentally determined, by applying Eq. (3) one obtains an experimental value of Θ which should consistently equal the conditional values that our theory predicts.
In principle, the entropic contribution of electrons gives an additional T^{2} correction owing to the bandstructure modification by thermal expansion^{16}. However, this correction to F is typically of parts in 10^{4} up to the highest temperature that quantum oscillations are observable^{8}. Frequency shifts with a T^{4} dependence have been observed for a few, nonmagnetic metals; these shifts were attributed to the lattice contribution to thermal expansion^{17,18}, as well as the electronphonon coupling^{19} [see supplementary note 2(A)]. Because of their distinct power law (T^{4}) compared to the topological and Sommerfeld corrections (T^{2}), lattice and electronphonon effects would in principle be easy to detect and analyze separately.
Next, we discuss the identification of band topology. Our approach senses the linearity of bands and hence the topological character needs to be inferred. As the argument is based on a k ⋅ p expansion, it is only applicable to small Fermi surfaces that are much smaller than the Brillouin zone. As topological materials of practical relevance generally host small Fermi pockets, this criterion is typically fulfilled. Even when linear bands with a small Fermi pocket are detected, a question remains about distinguishing massive from massless Dirac materials. Conservatively speaking, one can never completely rule out the possibility that any hypothesized Dirac fermion has a tiny mass m_{D} which leads to a weakly nonlinear energy dispersion \(E(k)=\pm \sqrt{{({v}_{x}\hslash {k}_{x})}^{2}+{({v}_{y}\hslash {k}_{y})}^{2}+{m}_{{{{{{\rm{D}}}}}}}^{2}}\) and \({{\Theta }}=(1/16) {E}_{{{{{{\rm{F}}}}}}} ( {E}_{{{{{{\rm{F}}}}}}} +2 {m}_{{{{{{\rm{D}}}}}}} )/{( {E}_{{{{{{\rm{F}}}}}}} + {m}_{{{{{{\rm{D}}}}}}} )}^{2}.\) The experimental uncertainty in Θ can be used to set an upper bound on ∣m_{D}∣. If the dispersion at the Fermi level is experimentally indistinguishable from a linear one, a hypothetical gap at the node is necessarily much smaller than the chemical potential (measured from the node), and has negligible influence on the lowenergy excitations. For example, graphene with a typical chemical potential (~meV) is well described by massless Dirac fermions, despite the existence of a spinorbitinduced gap (~μeV)^{20}.
High temperatures are natural opponents of quantum oscillations, because discontinuous changes in the occupation of Landau levels are smoothened out by the FermiDirac distribution, as illustrated in the top panel of Fig. 2. The characteristic T^{2} dependence for F is observable at a temperature scale T^{*} where 2π^{2}k_{B}T^{*} is comparable to the cyclotron energy, while for T ≫ T^{*} oscillations are exponentially suppressed by thermal damping^{8}. The optimal temperature window for observing F(T) is determined approximately by plotting the product (of the frequency shift and the amplitude) as a function of T, as in Fig. 2. Since T^{*} is inversely proportional to the effective mass m_{c}, the requirement for elevated temperatures does not preclude their observation even when quasiparticles masses are heavy, it simply reduces the optimal temperature window to lower values. For example, for m_{c} that is ten times the freeelectron mass, Fig. 2 predicts the optimal temperature window to be between 0.1 and 1 K. Our method hence is expected to apply to strongly interacting topological materials with strong mass renormalization. Detailed discussion on applicability to heavyfermion materials can be found in supplementary note 2(C).
Detection and analysis of temperaturedependent quantumoscillation frequency
Experimentally, these predictions turn out to be readily observable. Three distinct materials were analyzed (Fig. 3): (i) Cd_{3}As_{2} is a wellstudied prototypical Dirac semimetal with a timereversalrelated pair of Diractype Fermi pockets and no other pockets (F ≈ 43.7 T)^{21}. (ii) Bi_{2}O_{2}Se is a topologically trivial semimetal with a single, small electron pocket centered at Γ (F ≈ 33.3 T)^{22}. (iii) LaRhIn_{5} is a largecarrierdensity, multiband metal that hosts Brillouinzonesized pockets^{23} in addition to a very small pocket (F ≈ 6.9 T) that is inconsistent with conventional Schrödingerlike behavior^{24}. In their pioneering work, Mikitik and Sharlai proposed that the small pocket encloses a Dirac nodal line^{25}, based on an assumption that the spinorbit coupling is perturbatively weak. However, our firstprinciples calculation [detailed in Supplementary note 2(D) and supplementary note 4] suggest this assumption to be unjustified, leaving the topology of the small pocket still in question.
Crystalline microbars of (i–iii) for fourterminal resistivity measurements were prepared by Focused Ion Beam machining^{26}. These microbars feature optimized geometries for longitudinal transport and provide high signal amplitudes even in the highly conductive materials studied here. All samples show pronounced quantum oscillations of the longitudinal magnetoresistance, with a single small frequency in the lowfield regime (Fig. 3). We obtain F_{0}(E_{F}) from extrapolating the temperaturedependent oscillation frequency to zero temperature, and m_{c} from the temperature dependence of the amplitude. For each material, the temperature dependence of the frequency is obtained from fitting the entire experimental dataset [measured at different temperatures and fields (see Fig. 4)] to a single Lifshitz–Kosevich formula^{9}. The fitting is done by a standard least squares regression method using the nonlinear model fitting function provided by Mathematica, as detailed in supplementary note 3(A) and (B).
Both Cd_{3}As_{2} and Bi_{2}O_{2}Se are lowcarrierdensity materials in which the Sommerfeld correction applies, and accordingly a clear frequency shift, ΔF(T), is observed in both of them (Fig. 4). It is evident from the raw data that Cd_{3}As_{2} exhibits a stronger frequency shift compared to the trivial Bi_{2}O_{2}Se. For both cases, ΔF(T) falls directly onto the theoretical predictions \({{\Theta }}{(\pi {k}_{{{{{{\rm{B}}}}}}}T)}^{2}/{\beta }^{2}{F}_{0}({E}_{{{{{{\rm{F}}}}}}})\) from Eq. (3) for the trivial and topological case respectively. For Cd_{3}As_{2}, Θ = 5/48, as predicted for a Dirac semimetal with only two timereversalrelated Fermi pockets; for Bi_{2}O_{2}Se, Θ = 1/48 is consistent with a conventional semimetal with a single Fermi pocket. We emphasize that the coefficient of T^{2} has no tuning parameter as F_{0}(E_{F}) and m_{c} are fixed by measurement results, i.e., theory fixes Θ to take on different rational values depending on whether the pocket is Schrödinger or Dirac type.
In comparison, LaRhIn_{5} is a highcarrierdensity metal, and hence the measured ΔF(T) (for three devices) directly matches the prediction of Θ = 1/16, a purely topological correction. This confirms the small 7 T pocket of LaRhIn_{5} is Dirac type, with a chemical potential that is pinned by other large coexisting pockets.
The universal topological aspect of these distinct compounds becomes evident after subtracting the Sommerfeld correction described by supplementary Eq. (10) and (11) from the experimental ΔF for Bi_{2}O_{2}Se and Cd_{3}As_{2}. Remarkably, Cd_{3}As_{2} and all three devices of LaRhIn_{5} collapse on the same red line in Fig. 4c despite their highly different band structures and microscopic details, highlighting the common topological origin of ΔF^{top} and its insensitivity to materialspecific details. Instructively, a quantumoscillation phase analysis of Bi_{2}O_{2}Se and Cd_{3}As_{2} by the Landaufandiagram method uncovers a πphase shift in both of them (see Fig. 4d), despite their clearly distinct topology, exemplifying the faults of this method.
These results can be further quantitatively strengthened by the selfconsistency of ∣E_{F}∣ computed by two different ways. From k ⋅ p theory, it can be expressed in terms of the standard Lifshitz–Kosevich parameters: ∣E_{F}∣ = 2eℏF_{0}/m_{c} for the linearized Dirac pocket, and ∣E_{F}∣ = eℏF_{0}/m_{c} for the quadratic Schrödinger pocket. On the other hand, ∣E_{F}∣ can also be determined via ΔF(T): in the Dirac case, \( {E}_{{{{{{\rm{F}}}}}}} = \frac{\partial E}{\partial ({{{{{{\mathrm{log}}}}}}}\,{m}_{{{{{{\rm{c}}}}}}})}\) [cf. Eq. (1)] is deducible from the topological correction, while in the Schrödinger case ∣E_{F}∣ is deducible^{15} from the Sommerfeld correction to F. For the model correctly describing the topology of the pocket, both estimates for ∣E_{F}∣ should be consistent, and indeed this is what Table 1 shows. This allows for a simple selfconsistency check. By analyzing a measured temperaturedependent quantumoscillation frequency F(T) within both the Dirac/Weyl and Schrödinger framework, the match of both ∣E_{F}∣ signals the correct k ⋅ p model.
Discussions
To conclude, our experimental methodology allows us to diagnose the linear dispersion of small, topological Fermi pockets, as demonstrated by our three case studies. Despite their microscopic differences, all Dirac/Weyl/multifold fermions have a linear dispersion close to the nodal degeneracy. The linear dispersion is directly sensed by the temperature dependence of the oscillation frequency when the Fermi level is also close to the node. It is also capable of identifying multiWeyl fermions protected by crystallographic rotational symmetry, e.g., the dispersion of a double–Weyl (tripleWeyl) fermion is quadratic (cubic) in two momentum directions and linear in the third direction^{27}, hence they would be identifiable by measuring F(T) at various field orientations. Our methodology is applicable independent of the magnitude of the Zeeman splitting of Landau levels; this magnitude would affect the relative amplitudes of higher harmonics of quantum oscillations^{9} but not their frequency.
Because the energy scale for band inversion tends to be small compared to the bandwidth, topological Fermi pockets are often small compared to the Brillouin zone. It is not impossible for highly inverted materials that the dispersion of larger topological Fermi pockets acquires substantial nonlinear corrections, in which case our methodology becomes less useful for topological diagnosis. It is also less straightforward to subtract the Sommerfeld correction (from the frequency shift) in materials where a topological Fermi pocket coexists with a nontopological pocket of comparable size; here, supplementing our methodology with a firstprinciples calculation may be useful to isolate the topological frequency shift.
It will be interesting to apply our method to investigate the topology of Fermiliquid materials with extreme interactiondriven mass enhancement (e.g., heavyfermion materials), with the caveat that the optimal temperature for measuring F(T) is inversely proportional to the effective mass. The presence of Dirac fermions in LaRhIn_{5} suggests that the intimately related Ce(Co, Rh, Ir)In_{5} are prime candidates for such efforts. The Ce family has a similar band structure to LaRhIn_{5}, but are more prone to correlationdriven instabilities such as unconventional superconductivity^{28}. A different class of correlated topological metals include the Kondo–Weyl semimetals^{29,30}, in which itinerant electronic bands hybridize with localized (4f/5f)states leading to strongly renormalized Weyl dispersions.
As the field matures towards strongly interacting topological matter, it leaves the comfort zone in which abinitiopredicted topological band structures can straightforwardly be confirmed by angleresolved photoemission spectroscopy. The new conceptual and experimental challenges—arising from competing, neardegenerate ground states and unconventional superconductivity—call for new approaches to detect lowenergy excitations and assess their topological character. Extending the framework of quantum oscillations to topologically nontrivial Fermi surfaces, as presented here, will play a major role in this development.
Methods
Microstructure fabrication
Microdevices of all materials are fabricated with a FEI Helios Plasma FIB using Xeions. Thin slab (lamella) was dig out from a single crystalline material, which was transferred and glued down to a sapphire substrate. The transferred lamella was later patterned to the desired geometry with the Plasma FIB.
Bandstructure calculations
To check for the robustness of bandstructure results against choices of functionals in the calculation, the calculations were performed via two independent methods which are both detailedly described in supplementary note 4(A).
Data availability
Data that support the findings of this study are deposited to Zenodo with the access link: https://doi.org/10.5281/zenodo.5482689.
Code availability
Mathematica code used for the Lifshitz–Kosevich fit of temperaturedependent quantum oscillations can be found via the access link: https://doi.org/10.5281/zenodo.5482689.
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Acknowledgements
A.A. was supported initially by the Yale Postdoctoral Prize Fellowship, and subsequently by the Gordon and Betty Moore Foundation EPiQS Initiative through Grant No. GBMF 4305 and GBMF 8691 at the University of Illinois. S.Z, Q.W. and O.V.Y. acknowledge support by NCCR Marvel and the Swiss National Supercomputing Centre (CSCS) under Projects No. s832 and No. s1008. M.D.B. acknowledges studentship funding from EPSRC under grant no EP/L015110/1. E.D.B. and F.R. were supported by the U.S. DOE, Basic Energy Sciences, Division of Materials Sciences and Engineering. C.P. and P.J.W.M. acknowledge funding by the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (“MiTopMat”—grant agreement No. 715730). This project was funded by the Swiss National Science Foundation (Grants No. PP00P2_176789).
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Crystals were synthesized and characterized by F.R., E.D.B. (LaRhIn_{5}), T.T., H.P. (Bi_{2}O_{2}Se) and N.K., C.S., C.F. (Cd_{3}As_{2}). The experiment design, FIB microstructuring and the magnetotransport measurements were performed by C.G., C.P., A.E., K.R.S., M.B., P.J.W.M. A.A. developed, applied and described the theoretical framework, and the analysis of experimental results has been done by C.G. and C.P. Band structures were calculated by F.F., S.Z., Q.W., O.Y., C.F., and Y.S. All authors were involved in writing the paper.
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Guo, C., Alexandradinata, A., Putzke, C. et al. Temperature dependence of quantum oscillations from nonparabolic dispersions. Nat Commun 12, 6213 (2021). https://doi.org/10.1038/s41467021264501
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DOI: https://doi.org/10.1038/s41467021264501
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