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1.
J Am Chem Soc ; 145(8): 4527-4533, 2023 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-36789888

RESUMEN

Electrons in solids often adopt complex patterns of chemical bonding driven by the competition between energy gains from covalency and delocalization, and energy costs of double occupation to satisfy Pauli exclusion, with multiple intermediate states in the transition between highly localized, and magnetic, and delocalized, and nonmagnetic limits. Herein, we report a chemical pressure-driven transition from a proper Mn magnetic ordering phase transition to a Mn magnetic phase crossover in EuMn2P2 the limiting end member of the EuMn2X2 (X = Sb, As, P) family of layered materials. This loss of a magnetic ordering occurs despite EuMn2P2 remaining an insulator at all temperatures, and with a phase transition to long-range Eu antiferromagnetic order at TN ≈ 17 K. The absence of a Mn magnetic phase transition contrasts with the formation of long-range Mn order at T ≈ 130 K in isoelectronic EuMn2Sb2 and EuMn2As2. Temperature-dependent specific heat and 31P NMR measurements provide evidence for the development of short-range Mn magnetic correlations from T ≈ 250-100 K, interpreted as a precursor to covalent bond formation. Density functional theory calculations demonstrate an unusual sensitivity of the band structure to the details of the imposed Mn and Eu magnetic order, with an antiferromagnetic Mn arrangement required to recapitulate an insulating state. Our results imply a picture in which long-range Mn magnetic order is suppressed by chemical pressure, but that antiferromagnetic correlations persist, narrowing bands and producing an insulating state.

2.
Nat Mater ; 22(1): 58-63, 2023 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-36411349

RESUMEN

Quantum spin liquids (QSLs) are topologically ordered states of matter that host fractionalized excitations. A particular route towards a QSL is via strongly bond-dependent interactions on the hexagonal lattice. A number of Ru- and Ir-based candidate Kitaev QSL materials have been pursued, but all have appreciable non-Kitaev interactions. Using time-domain terahertz spectroscopy, we observed a broad magnetic continuum over a wide range of temperatures and fields in the honeycomb cobalt-based magnet BaCo2(AsO4)2, which has been proposed to be a more ideal version of a Kitaev QSL. Applying an in-plane magnetic field of ~0.5 T suppresses the magnetic order, and at higher fields, applying the field gives rise to a spin-polarized state. Under a 4 T magnetic field that was oriented principally out of plane, a broad magnetic continuum was observed that may be consistent with a field-induced QSL. Our results indicate BaCo2(AsO4)2 is a promising QSL candidate.

3.
Sci Adv ; 7(16)2021 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-33863734

RESUMEN

The linear band crossings of 3D Dirac and Weyl semimetals are characterized by a charge chirality, the parallel or antiparallel locking of electron spin to its momentum. These materials are believed to exhibit an E · B chiral magnetic effect that is associated with the near conservation of chiral charge. Here, we use magneto-terahertz spectroscopy to study epitaxial Cd3As2 films and extract their conductivities σ(ω) as a function of E · B. As field is applied, we observe a markedly sharp Drude response that rises out of the broader background. Its appearance is a definitive signature of a new transport channel and consistent with the chiral response, with its spectral weight a measure of the net chiral charge and width a measure of the scattering rate between chiral species. The field independence of the chiral relaxation establishes that it is set by the approximate conservation of the isospin that labels the crystalline point-group representations.

4.
Phys Rev Lett ; 127(26): 267201, 2021 Dec 24.
Artículo en Inglés | MEDLINE | ID: mdl-35029479

RESUMEN

We observe a wealth of multimagnon bound states in the strongly anisotropic spin-1 triangular antiferromagnet FeI_{2} using time-domain terahertz spectroscopy. These unconventional excitations can arise in ordered magnets due to attractive magnon-magnon interactions and alter their properties. We analyze the energy-magnetic field spectrum via an exact diagonalization method for a dilute gas of interacting magnons and detect up to 4- and 6-magnon bound states, hybridized with single magnons. This zoo of tunable interacting quasiparticles provides a unique platform to study decay and renormalization, reminiscent of the few-body problems found in cold-atom, nuclear, and particle physics.

5.
Phys Rev Lett ; 125(21): 217401, 2020 Nov 20.
Artículo en Inglés | MEDLINE | ID: mdl-33274990

RESUMEN

SrRuO_{3}, a ferromagnet with an approximately 160 K Curie temperature, exhibits a T^{2}-dependent dc resistivity below ≈30 K. Nevertheless, previous optical studies in the infrared and terahertz range show non-Drude dynamics at low temperatures, which seem to contradict Fermi-liquid predictions. In this work, we measure the low-frequency THz range response of thin films with residual resistivity ratios, ρ_{300K}/ρ_{4K}≈74. At temperatures below 30 K, we find both a sharp zero frequency mode which has a width narrower than k_{B}T/ℏ as well as a broader zero frequency Lorentzian that has at least an order of magnitude larger scattering. Both features have temperature dependences consistent with a Fermi liquid with the wider feature explicitly showing a T^{2} scaling. Above 30 K, there is a crossover to a regime described by a single Drude peak that we believe arises from strong interband electron-electron scattering. Such two channel Drude transport sheds light on reports of the violation of Matthiessen's rule and extreme sensitivity to disorder in metallic ruthenates.

6.
Nano Lett ; 20(8): 5991-5996, 2020 Aug 12.
Artículo en Inglés | MEDLINE | ID: mdl-32633978

RESUMEN

We investigated the magnetoterahertz response of the Dirac semimetal Cd3As2 and observed a particularly low frequency optical phonon as well as a very prominent and field-sensitive cyclotron resonance. As the cyclotron frequency is tuned with the field to pass through the phonon, the phonon becomes circularly polarized, as shown by a notable splitting in its response to right- and left-hand polarized light. This splitting can be expressed as an effective phonon magnetic moment that is approximately 2.7 times the Bohr magneton, which is almost 4 orders of magnitude larger than ab initio calculations predict for phonon magnetic moments in nonmagnetic insulators. This exceedingly large value is due to the coupling of the phonons to the cyclotron motion and is controlled directly by the electron-phonon coupling constant. This field-tunable circular-polarization-selective coupling provides new functionality for nonlinear optics to create light-induced topological phases in Dirac semimetals.

7.
Phys Rev Lett ; 124(11): 117402, 2020 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-32242712

RESUMEN

We report strong terahertz (∼10^{12} Hz) high harmonic generation at room temperature in thin films of Cd_{3}As_{2}, a three-dimensional Dirac semimetal. Third harmonics are detectable with a tabletop light source and can be as strong as 100 V/cm by applying a fundamental field of 6.5 kV/cm inside the film, demonstrating an unprecedented efficiency for terahertz frequency conversion. Our time-resolved terahertz spectroscopy and calculations also clarify the microscopic mechanism of the nonlinearity originating in the coherent acceleration of Dirac electrons in momentum space. Our results provide clear insights for nonlinear currents of Dirac electrons driven by the terahertz field under the influence of scattering, paving the way toward novel devices for high-speed electronics and photonics based on topological semimetals.

8.
Phys Rev Lett ; 124(3): 037203, 2020 Jan 24.
Artículo en Inglés | MEDLINE | ID: mdl-32031844

RESUMEN

NiNb_{2}O_{6} is an almost ideal realization of a 1D spin-1 ferromagnetic Heisenberg chain compound with weak unidirectional anisotropy. Using time-domain THz spectroscopy, we measure the low-energy electrodynamic response of NiNb_{2}O_{6} as a function of temperature and external magnetic field. At low temperatures, we find a magnonlike spin excitation, which corresponds to the lowest energy excitation at q∼0. At higher temperatures, we unexpectedly observe a temperature-dependent renormalization of the spin-excitation energy, which has a strong dependence on field direction. Using theoretical arguments, exact diagonalizations, and finite temperature dynamical Lanczos calculations, we construct a picture of magnon-magnon interactions that naturally explains the observed renormalization. We show how magnetic field strength and direction may be used to directly tune the sign of the magnon-magnon interaction. This unique scenario is a consequence of the spin-1 nature and has no analog in the more widely studied spin-1/2 systems.

9.
Nat Commun ; 11(1): 909, 2020 Feb 14.
Artículo en Inglés | MEDLINE | ID: mdl-32060261

RESUMEN

Antiferromagnetic spin motion at terahertz (THz) frequencies attracts growing interests for fast spintronics, however, their smaller responses to external field inhibit device application. Recently the noncollinear antiferromagnet Mn3Sn, a Weyl semimetal candidate, was reported to show large anomalous Hall effect (AHE) at room temperature comparable to ferromagnets. Dynamical aspect of such large responses is an important issue to be clarified for future THz data processing. Here the THz anomalous Hall conductivity in Mn3Sn thin films is investigated by polarization-resolved spectroscopy. Large anomalous Hall conductivity [Formula: see text] at THz frequencies is clearly observed as polarization rotation. A peculiar temperature dependence corresponding to the breaking/recovery of symmetry in the spin texture is also discussed. Observation of the THz AHE at room temperature demonstrates the ultrafast readout for the antiferromagnetic spintronics using Mn3Sn, and will also open new avenue for studying nonequilibrium dynamics in Weyl antiferromagnets.

10.
Phys Rev Lett ; 122(25): 257401, 2019 Jun 28.
Artículo en Inglés | MEDLINE | ID: mdl-31347881

RESUMEN

We show that the new technique of terahertz 2D coherent spectroscopy is capable of giving qualitatively new information about fractionalized spin systems. For the prototypical example of the transverse field Ising chain, we demonstrate theoretically that, despite the broad continuum of excitations in linear response, the 2D spectrum contains sharp features that are a coherent signature of a "spinon echo," which gives previously inaccessible information such as the lifetime of the two-spinon excited state. The effects of disorder and finite lifetime, which are practically indistinguishable in the linear optical or neutron response, manifest in dramatically different fashion in the 2D spectra. Our results may be directly applicable to model quasi-1D transverse field Ising chain systems such as CoNb_{2}O_{6}, but the concept can be applied to fractionalized spin systems in general.

11.
Phys Rev Lett ; 122(1): 017002, 2019 Jan 11.
Artículo en Inglés | MEDLINE | ID: mdl-31012661

RESUMEN

Epitaxial bilayer films of Bi(110) and Ni host a time-reversal symmetry breaking superconducting order with an unexpectedly high transition temperature T_{c}=4.1 K. Using time-domain THz spectroscopy, we measure the low energy electrodynamic response of a Bi/Ni bilayer thin film from 0.2 to 2 THz as a function of temperature and magnetic field. We analyze the data in the context of a Bardeen-Cooper-Schrieffer-like superconductor with a finite normal-state scattering rate. In a zero magnetic field, all states in the film become fully gapped, providing important constraints into possible pairing symmetries. Our data appear to rule out the odd-frequency pairing that is natural for many ferromagnetic-superconductor interfaces. By analyzing the magnetic field-dependent response in terms of a pair-breaking parameter, we determine that superconductivity develops over the entire bilayer sample which may point to the p-wave like nature of unconventional superconductivity.

12.
Phys Rev Lett ; 122(9): 097401, 2019 Mar 08.
Artículo en Inglés | MEDLINE | ID: mdl-30932532

RESUMEN

Pb_{1-x}Sn_{x}Te has been shown to be an interesting tunable topological crystalline insulator system. We present a magnetoterahertz spectroscopic study of thin films of Pb_{0.5}Sn_{0.5}Te. The complex Faraday rotation angle and optical conductivity in the circular basis are extracted without any additional assumptions. Our quantitative measures of the THz response allow us to show that the sample studied contains two types of bulk carriers. One is p type and originates in 3D Dirac bands. The other is n type and appears to be from more conventional 3D bands. These two types of carriers display different cyclotron resonance dispersions. Through simulating the cyclotron resonance of hole carriers, we can determine the Fermi energy and Fermi velocity. Furthermore, the scattering rates of p-type and n-type carriers were found to show opposite field dependences, which can be attributed to their different Landau level broadening behaviors under magnetic field. Our work provides a new way to isolate real topological signatures of bulk states in Dirac and Weyl semimetals.

13.
Phys Rev Lett ; 122(2): 027003, 2019 Jan 18.
Artículo en Inglés | MEDLINE | ID: mdl-30720319

RESUMEN

Overdoped high-temperature cuprate superconductors have often been understood within the standard BCS framework of superconductivity. However, measurements in a variety of overdoped cuprates indicate that the superfluid density is much smaller than expected from BCS theory and decreases smoothly to zero as the doping is increased. Here, we combine time-domain THz spectroscopy with kHz range mutual inductance measurements on the same overdoped La_{2-x}Sr_{x}CuO_{4} films to determine the total, superfluid, and uncondensed spectral weight as a function of doping. A significant fraction of the carriers remains uncondensed in a wide Drude-like peak as T→0, while the superfluid density remains linear in temperature. These observations are seemingly inconsistent with existing, realistic theories of impurity scattering suppressing the superfluid density in a BCS-like d-wave superconductor. Our large measurement frequency range gives us a unique look at the low frequency spectral weight distribution, which may suggest the presence of quantum phase fluctuations as the critical doping is approached.

14.
Phys Rev Lett ; 120(16): 167002, 2018 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-29756920

RESUMEN

It is observed that many thin superconducting films with not too high disorder level (generally R_{N}/□<2000 Ω) placed in magnetic field show an anomalous metallic phase where the resistance is low but still finite as temperature goes to zero. Here we report in weakly disordered amorphous InO_{x} thin films that this anomalous metal phase possesses no cyclotron resonance and hence non-Drude electrodynamics. The absence of a finite frequency resonant mode can be associated with a vanishing downstream component of the vortex current parallel to the supercurrent and an emergent particle-hole symmetry of this metal, which establishes its non-Fermi-liquid character.

15.
J Water Sanit Hyg Dev ; 8(3): 429-438, 2018 Apr 18.
Artículo en Inglés | MEDLINE | ID: mdl-33384867

RESUMEN

This paper discusses the need to incorporate equity assessment into the planning and monitoring of sanitation service delivery to South African informal settlements. Equity assessment criteria were drawn from literature and a study of sanitation service delivery to informal settlements in three South African municipalities (Cape Town, Johannesburg and eThekwini) over the period 2012-2015. Three key dimensions of equity - resource allocation, access and stakeholder perceptions - were identified. These had eight associated criteria: (1) funds allocated for basic sanitation, (2) number of staff allocated to informal settlements, (3) disparities in access, (4) proportion of functioning sanitation facilities, (5) menstrual hygiene management (MHM) inclusion, (6) access to information, (7) meets users' notions of dignity, and (8) integration of the perspectives of key stakeholders. Key findings of the study indicate that the current focus on reducing service backlogs largely ignores equity and there is a need to better address this through the incorporation of: equity assessments, improving access to information, and the inclusion of marginalised communities in the planning of sanitation services.

16.
Nat Commun ; 8(1): 2097, 2017 12 13.
Artículo en Inglés | MEDLINE | ID: mdl-29235469

RESUMEN

Dirac and Weyl semimetals with linearly crossing bands are the focus of much recent interest in condensed matter physics. Although they host fascinating phenomena, their physics can be understood in terms of weakly interacting electrons. In contrast, more than 40 years ago, Abrikosov pointed out that quadratic band touchings are generically strongly interacting. We have performed terahertz spectroscopy on the films of the conducting pyrochlore Pr2Ir2O7, which has been shown to host a quadratic band touching. A dielectric constant as large as [Formula: see text] is observed at low temperatures. In such systems, the dielectric constant is a measure of the relative scale of interactions, which are therefore in our material almost two orders of magnitude larger than the kinetic energy. Despite this, the scattering rate exhibits a T 2 dependence, which shows that for finite doping a Fermi liquid state survives-however, with a scattering rate close to the maximal value allowed.

17.
Phys Rev Lett ; 119(22): 227601, 2017 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-29286798

RESUMEN

The symmetric splitting of two spin-wave branches in an antiferromagnetic resonance (AFR) experiment has been an essential measurement of antiferromagnets for over half a century. In this work, circularly polarized time-domain THz spectroscopy experiments performed on the low symmetry multiferroic hexagonal HoMnO_{3} reveal an AFR of the Mn sublattice to split asymmetrically in an applied magnetic field, with an ≈50% difference in g factors between the high and low energy branches of this excitation. The temperature dependence of the g factors, including a drastic renormalization at the Ho spin ordering temperature, reveals this asymmetry to unambiguously stem from Ho-Mn interactions. Theoretical calculations demonstrate that the AFR asymmetry is not explained by conventional Ho-Mn exchange mechanisms alone and is only reproduced if quartic spin interactions are also included in the spin Hamiltonian. Our results provide a paradigm for the optical study of such novel interactions in hexagonal manganites and low symmetry antiferromagnets in general.

18.
Science ; 354(6316): 1124-1127, 2016 12 02.
Artículo en Inglés | MEDLINE | ID: mdl-27934759

RESUMEN

Topological insulators have been proposed to be best characterized as bulk magnetoelectric materials that show response functions quantized in terms of fundamental physical constants. Here, we lower the chemical potential of three-dimensional (3D) Bi2Se3 films to ~30 meV above the Dirac point and probe their low-energy electrodynamic response in the presence of magnetic fields with high-precision time-domain terahertz polarimetry. For fields higher than 5 tesla, we observed quantized Faraday and Kerr rotations, whereas the dc transport is still semiclassical. A nontrivial Berry's phase offset to these values gives evidence for axion electrodynamics and the topological magnetoelectric effect. The time structure used in these measurements allows a direct measure of the fine-structure constant based on a topological invariant of a solid-state system.

19.
Phys Rev Lett ; 117(13): 136401, 2016 Sep 23.
Artículo en Inglés | MEDLINE | ID: mdl-27715109

RESUMEN

We report on optical reflectivity experiments performed on Cd_{3}As_{2} over a broad range of photon energies and magnetic fields. The observed response clearly indicates the presence of 3D massless charge carriers. The specific cyclotron resonance absorption in the quantum limit implies that we are probing massless Kane electrons rather than symmetry-protected 3D Dirac particles. The latter may appear at a smaller energy scale and are not directly observed in our infrared experiments.

20.
Phys Rev Lett ; 115(21): 217602, 2015 Nov 20.
Artículo en Inglés | MEDLINE | ID: mdl-26636873

RESUMEN

We have utilized time-domain magnetoterahertz spectroscopy to investigate the low-frequency optical response of the topological insulator Cu_{0.02}Bi_{2}Se_{3} and Bi_{2}Se_{3} films. With both field and frequency dependence, such experiments give sufficient information to measure the mobility and carrier density of multiple conduction channels simultaneously. We observe sharp cyclotron resonances (CRs) in both materials. The small amount of Cu incorporated into the Cu_{0.02}Bi_{2}Se_{3} induces a true bulk insulator with only a single type of conduction with a total sheet carrier density of ~4.9×10^{12}/cm^{2} and mobility as high as 4000 cm^{2}/V·s. This is consistent with conduction from two virtually identical topological surface states (TSSs) on the top and bottom of the film with a chemical potential ~145 meV above the Dirac point and in the bulk gap. The CR broadens at high fields, an effect that we attribute to an electron-phonon interaction. This assignment is supported by an extended Drude model analysis of the zero-field Drude conductance. In contrast, in normal Bi_{2}Se_{3} films, two conduction channels were observed, and we developed a self-consistent analysis method to distinguish the dominant TSSs and coexisting trivial bulk or two-dimensional electron gas states. Our high-resolution Faraday rotation spectroscopy on Cu_{0.02}Bi_{2}Se_{3} paves the way for the observation of quantized Faraday rotation under experimentally achievable conditions to push the chemical potential in the lowest Landau level.

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