arXiv subjects

Matthew D. Watson

Publications and source records attributed to Matthew D. Watson.

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arXiv2022

FeSe and the missing electron pocket problem

The nature and origin of electronic nematicity remains a significant challenge in our understanding of the iron-based superconductors. This is particularly evident in the iron chalcogenide, FeSe, where it is currently unclear how the experimentally determined Fermi surface near the M point evolves from having two electron pockets in the tetragonal state to exhibiting just a single electron pocket in the nematic state. This has posed a major theoretical challenge, which has become known as the missing electron pocket problem of FeSe, and is of central importance if we wish to uncover the secrets behind nematicity and superconductivity in the wider iron-based superconductors. Here, we review the recent experimental work uncovering this nematic Fermi surface of FeSe from both ARPES and STM measurements, as well as current theoretical attempts to explain this missing electron pocket of FeSe, with a particular focus on the emerging importance of incorporating the $d_{xy}$ orbital into theoretical descriptions of the nematic state. Furthermore, we will discuss the consequence this missing electron pocket has on the theoretical understanding of superconductivity in this system and present several remaining open questions and avenues for future research.

cond-mat.supr-con↗

arXiv2021

Fermiology and electron-phonon coupling in the 2H and 3R polytypes of NbS$\boldsymbol{_2}$

We investigate the electronic structure of the 2H and 3R polytypes of NbS$_2$. The Fermi surfaces measured by angle-resolved photoemission spectroscopy show a remarkable difference in size, reflecting a significantly increased band filling in 3R-Nb$_{1+x}$S$_2$ compared to 2H-NbS$_2$, which we attribute to the presence of additional interstitial Nb which act as electron donors. Thus we find that the stoichiometry, rather than the stacking arrangement, is the most important factor in the difference in electronic and physical properties of the two phases. Our high resolution data on the 2H phase shows kinks in the spectral function that are fingerprints of the electron-phonon coupling. However, the strength of the coupling is found to be much larger for the the sections of bands with Nb 4$d_{x^2-y^2,xy}$ character than for the Nb 4$d_{3z^2-r^2}$. Our results provide an experimental framework for interpreting the two-gap superconductivity and "latent" charge density wave in 2H-NbS$_2$.

cond-mat.supr-con↗

arXiv2020

Bulk and surface electronic states in the dosed semimetallic HfTe$\boldsymbol{_2}$

The dosing of layered materials with alkali metals has become a commonly used strategy in ARPES experiments. However, precisely what occurs under such conditions, both structurally and electronically, has remained a matter of debate. Here we perform a systematic study of 1T-HfTe$_2$, a prototypical semimetal of the transition metal dichalcogenide family. By utilizing photon energy-dependent angle-resolved photoemission spectroscopy (ARPES), we have investigated the electronic structure of this material as a function of Potassium (K) deposition. From the k$_z$ maps, we observe the appearance of 2D dispersive bands after electron dosing, with an increasing sharpness of the bands, consistent with the wavefunction confinement at the topmost layer. In our highest-dosing cases, a monolayer-like electronic structure emerges, presumably as a result of intercalation of the alkali metal. Here, by bringing the topmost valence band below $E_F$, we can directly measure a band overlap of $\sim$ 0.2 eV. However, 3D bulk-like states still contribute to the spectra even after considerable dosing. Our work provides a reference point for the increasingly popular studies of the alkali metal dosing of semimetals using ARPES.

cond-mat.mtrl-sci↗

arXiv2020

Revealing the single electron pocket of FeSe in a single orthorhombic domain

We measure the electronic structure of FeSe from within individual orthorhombic domains. Enabled by an angle-resolved photoemission spectroscopy beamline with a highly focused beamspot (nano-ARPES), we identify clear stripe-like orthorhombic domains in FeSe with a length scale of approximately 1-5~$μ$m. Our photoemission measurements of the Fermi surface and band structure within individual domains reveal a single electron pocket at the Brillouin zone corner. This result provides clear evidence for a one-electron pocket electronic structure of FeSe, observed without the application of uniaxial strain, and calls for further theoretical insight into this unusual Fermi surface topology. Our results also showcase the potential of nano-ARPES for the study of correlated materials with local domain structures.

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arXiv2020

Band hybridisation at the semimetal-semiconductor transition of Ta$_2$NiSe$_5$ enabled by mirror-symmetry breaking

We present a combined study from angle-resolved photoemission and density-functional theory calculations of the temperature-dependent electronic structure in the excitonic insulator candidate Ta$_2$NiSe$_5$. Our experimental measurements unambiguously establish the normal state as a semimetal with a significant band overlap of $>$100~meV. Our temperature-dependent measurements indicate how these low-energy states hybridise when cooling through the well-known 327~K phase transition in this system. From our calculations and polarisation-dependent photoemission measurements, we demonstrate the importance of a loss of mirror symmetry in enabling the band hybridisation, driven by a shear-like structural distortion which reduces the crystal symmetry from orthorhombic to monoclinic. Our results thus point to the key role of the lattice distortion in enabling the phase transition of Ta$_2$NiSe$_5$.

cond-mat.str-el↗

arXiv2019

Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe$_3$

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe$_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through ${T_\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te ${5p}$ and the Cr ${e_g}$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr ${t_{2g}}$ states that carry the majority of the spin moment. The ${t_{2g}}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

cond-mat.str-el↗

arXiv2019

Fermi-crossing Type-II Dirac fermions and topological surface states in NiTe2

Transition-metal dichalcogenides (TMDs) offer an ideal platform to experimentally realize Dirac fermions. However, typically these exotic quasiparticles are located far away from the Fermi level, limiting the contribution of Dirac-like carriers to the transport properties. Here we show that NiTe2 hosts both bulk Type-II Dirac points and topological surface states. The underlying mechanism is shared with other TMDs and based on the generic topological character of the Te p-orbital manifold. However, unique to NiTe2, a significant contribution of Ni d orbital states shifts the energy of the Type-II Dirac point close to the Fermi level. In addition, one of the topological surface states intersects the Fermi energy and exhibits a remarkably large spin splitting of 120 meV. Our results establish NiTe2 as an exciting candidate for next-generation spintronics devices.

cond-mat.mtrl-sci↗

arXiv2019

$k_z$ selective scattering within Quasiparticle Interference measurements of FeSe

Quasiparticle interference (QPI) provides a wealth of information relating to the electronic structure of a material. However, it is often assumed that this information is constrained to two-dimensional electronic states. Here, we show that this is not necessarily the case. For FeSe, a system dominated by surface defects, we show that it is actually all electronic states with negligible group velocity in the $z$ axis that are contained within the experimental data. By using a three-dimensional tight binding model of FeSe, fit to photoemission measurements, we directly reproduce the experimental QPI scattering dispersion, within a T-matrix formalism, by including both $k_z = 0$ and $k_z = π$ electronic states. This result unifies both tunnelling and photoemission based experiments on FeSe and highlights the importance of $k_z$ within surface sensitive measurements of QPI.

cond-mat.supr-con↗

arXiv2019

On the origin of the anomalous peak in the resistivity of TiSe$_2$

Resistivity measurements of TiSe$_2$ typically show only a weak change in gradient at the charge density wave transition at $T_{CDW}\approx$ 200~K, but more prominently feature a broad peak at a lower $T_{peak}\sim$ 165~K, which has remained poorly understood despite decades of research on the material. Here we present quantitative simulations of the resistivity using a simplified parametrization of the normal state band structure, based on recent photoemission data. Our simulations reproduce the overall profile of the resistivity of TiSe$_2$, including its prominent peak, without implementing the CDW at all. We find that the peak in resistivity corresponds to a crossover between a low temperature regime with electron-like carriers only, to a regime around room temperature where thermally activated and highly mobile hole-like carriers dominate the conductivity. Even when implementing substantial modifications to model the CDW below the transition temperature, we find that these thermal population effects still dominate the transport properties of TiSe$_2$.

cond-mat.str-el↗

arXiv2019

Probing the reconstructed Fermi surface of antiferromagnetic BaFe$_2$As$_2$ in one domain

We revisit the electronic structure of BaFe$_2$As$_2$, the archetypal parent compound of the Fe-based superconductors, using angle-resolved photoemission spectroscopy (ARPES). Our high-resolution measurements of samples detwinned by the application of a mechanical strain reveal a highly anisotropic 3D Fermi surface in the low temperature magnetic phase. By comparison of the observed dispersions with ab-initio calculations, we argue that overall it is magnetism, rather than orbital ordering, which is the dominant effect, reconstructing the electronic structure across the Fe 3d bandwidth. Finally, we measure band dispersions directly from within one domain without applying strain to the sample, by using the sub-micron focused beam spot of a nano-ARPES instrument.

cond-mat.supr-con↗

arXiv2019

Orbital- and $k_z$-selective hybridisation of Se 4p and Ti 3d states in the charge density wave phase of TiSe$_2$

We revisit the enduring problem of the $2\times{}2\times{}2$ charge density wave (CDW) order in TiSe$_2$, utilising photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridisation that is strongly $k_z$-dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe$_2$.

cond-mat.str-el↗

arXiv2018

Scaling of the superconducting gap with orbital character in FeSe

We use high-resolution angle-resolved photoemission spectroscopy to map the three-dimensional momentum dependence of the superconducting gap in FeSe. We find that on both the hole and electron Fermi surfaces, the magnitude of the gap follows the distribution of $d_{yz}$ orbital weight. Furthermore, we theoretically determine the momentum dependence of the superconducting gap by solving the linearized gap equation using a tight binding model which quantitatively describes both the experimental band dispersions and orbital characters. By considering a Fermi surface only including one electron pocket, as observed spectroscopically, we obtain excellent agreement with the experimental gap structure. Our finding of a scaling between the superconducting gap and the $d_{yz}$ orbital weight supports the interpretation of superconductivity mediated by spin-fluctuations in FeSe.

cond-mat.supr-con↗

arXiv2017

Disorder quenching of the Charge Density Wave in ZrTe3

The charge density wave (CDW) in ZrTe3 is quenched in samples with small amount of Te iso-electronically substituted by Se. Using angle-resolved photoemission spectroscopy we observe subtle changes in the electronic band dispersions and Fermi surfaces on Se substitution. The scattering rates are substantially increased, in particular for the large three-dimensional Fermi surface sheet. The quasi-one-dimensional band is unaffected by the substitution and still shows a gap at low temperature, which starts to open from room temperature. The detailed temperature dependence reveals that the long-range order is absent in the electronic states as in the periodic lattice distortion. The competition between superconductivity and CDW is thus linked to the suppression of long-range order of the CDW.

cond-mat.supr-con↗

arXiv2017

The three-dimensional electronic structure of the nematic and antiferromagnetic phases of NaFeAs from detwinned ARPES measurements

We report a comprehensive ARPES study of NaFeAs, a prototypical parent compound of the Fe-based superconductors. By mechanically detwinning the samples, we show that in the nematic phase (below the structural transition at $T_s$ = 54 K but above the antiferromagnetic transition at $T_N$ = 43 K) spectral weight is detected on only the elliptical electron pocket along the longer $a_{orth}$ axis. This dramatic anisotropy is likely to arise as a result of coupling to a fluctuating antiferromagnetic order in the nematic phase. In the long-range ordered antiferromagnetic state below $T_N$, this single electron pocket is backfolded and hybridises with the hole bands, leading to the reconstructed Fermi surface. By careful analysis of the $k_z$ variation, we show that the backfolding of spectral weight in the magnetic phase has a wavector of ($π$,0,$π$), with the $c$-axis component being in agreement with the magnetic ordering in NaFeAs observed by neutron scattering. Our results clarify the origin of the tiny Fermi surfaces of NaFeAs at low temperatures and highlight the importance of the three-dimensional aspects of the electronic and magnetic properties of Fe-based superconductors.

cond-mat.supr-con↗

arXiv2017

Emergence of Dirac-like bands in the monolayer limit of epitaxial Ge films on Au(111)

After the discovery of Dirac fermions in graphene, it has become a natural question to ask whether it is possible to realize Dirac fermions in other two-dimensional (2D) materials as well. In this work, we report the discovery of multiple Dirac-like electronic bands in ultrathin Ge films grown on Au(111) by angle-resolved photoelectron spectroscopy. By tuning the thickness of the films, we are able to observe the evolution of their electronic structure when passing through the monolayer limit. Our discovery may signify the synthesis of germanene, a 2D honeycomb structure made of Ge, which is a promising platform for exploring exotic topological phenomena and enabling potential applications.

cond-mat.mtrl-sci↗

arXiv2017

The key ingredients of the electronic structure of FeSe

FeSe is a fascinating superconducting material at the frontier of research in condensed matter physics. Here we provide an overview on the current understanding of the electronic structure of FeSe, focusing in particular on its low energy electronic structure as determined from angular resolved photoemission spectroscopy, quantum oscillations and magnetotransport measurements of single crystal samples. We discuss the unique place of FeSe amongst iron-based superconductors, being a multi-band system exhibiting strong orbitally-dependent electronic correlations and unusually small Fermi surfaces, prone to different electronic instabilities. We pay particular attention to the evolution of the electronic structure which accompanies the tetragonal-orthorhombic structural distortion of the lattice around 90 K, which stabilizes a unique nematic electronic state. Finally, we discuss how the multi-band multi-orbital nematic electronic structure has an impact on the understanding of the superconductivity, and show that the tunability of the nematic state with chemical and physical pressure will help to disentangle the role of different competing interactions relevant for enhancing superconductivity.

cond-mat.supr-con↗

arXiv2017

Shifts and Splittings of the Hole Bands in the Nematic Phase of FeSe

We report a high-resolution laser-based angle-resolved photoemission spectroscopy (laser-ARPES) study of single crystals of FeSe, focusing on the temperature-dependence of the hole-like bands around the ${\rm Γ}$ point. As the system cools through the tetragonal-orthorhombic "nematic" structural transition at 90~K, the splitting of the $d_{xz}$/$d_{yz}$ bands is observed to increase by a magnitude of 13 meV. Moreover, the onset of a $\sim$10 meV downward shift of the $d_{xy}$ band is also at 90~K. These measurements provide clarity on the nature, magnitude and temperature-dependence of the band shifts at the ${\rm Γ}$ point in the nematic phase of FeSe.

cond-mat.supr-con↗

arXiv2016

Formation of Hubbard-like bands as a fingerprint of strong electron-electron interactions in FeSe

We use angle-resolved photo-emission spectroscopy (ARPES) to explore the electronic structure of single crystals of FeSe over a wide range of binding energies and study the effects of strong electron-electron correlations. We provide evidence for the existence of "Hubbard-like bands" at high binding energies consisting of incoherent many-body excitations originating from Fe $3d$ states in addition to the renormalized quasiparticle bands near the Fermi level. Many high energy features of the observed ARPES data can be accounted for when incorporating effects of strong local Coulomb interactions in calculations of the spectral function via dynamical mean-field theory, including the formation of a Hubbard-like band. This shows that over the energy scale of several eV, local correlations arising from the on-site Coulomb repulsion and Hund's coupling are essential for a proper understanding of the electronic structure of FeSe and other related iron based superconductors.

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