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Single-photon emitters serve as building blocks for many emerging concepts in quantum photonics. The recent identification of bright, tunable, and stable emitters in hexagonal boron nitride (hBN) has opened the door to quantum platforms operating across the infrared to ultraviolet spectrum. While it is widely acknowledged that defects are responsible for single-photon emitters in hBN, crucial details regarding their origin, electronic levels, and orbital involvement remain unknown. Here, we employ a combination of resonant inelastic X-ray scattering and photoluminescence spectroscopy in defective hBN unveiling an elementary excitation at 285 meV that gives rise to a plethora of harmonics correlated with single-photon emitters. We discuss the importance of N $\pi^*$ antibonding orbitals in shaping the electronic states of the emitters. The discovery of the elementary excitations of hBN provides new fundamental insights into quantum emission in low-dimensional materials, paving the way for future investigations in other platforms.

An experimental determination of electronic phase diagrams of high-transition temperature (high-$T_c$) superconductors forms the basis for a microscopic understanding of unconventional superconductivity. For most high-$T_c$ superconductors, the electronic phase diagrams are established through partial chemical substitution, which also induces lattice disorder. Here we show that symmetry-specific uniaxial strain can be used to study electronic phases in iron-based superconductors, composed of two-dimensional nearly square iron lattice planed separated by other elements. By applying tunable uniaxial strain along different high symmetry directions and carrying out transport measurements, we establish strain-tuning dependent electronic nematicity, antiferromagnetic (AF) order, and superconductivity of BaFe$_2$(As$_{1-x}$P$_{x}$)$_2$ superconductor. We find that uniaxial strain along the nearest Fe-Fe direction can dramatically tune the AF order and superconductivity, producing an electronic phase diagram clearly different from the chemical substitution-induced one. Our results thus establish strain tuning as a way to study the intertwined orders in correlated electron materials without using chemical substitution.

Kagome metals are widely recognized as versatile platforms for exploring novel topological properties, unconventional electronic correlations, magnetic frustration, and superconductivity. In the $R$V$_6$Sn$_6$ family of materials ($R$ = Sc, Y, Lu), ScV$_6$Sn$_6$ hosts an unusual charge density wave ground state as well as structural similarities with the $A$V$_3$Sb$_5$ system ($A$ = K, Cs, Rb). In this work, we combine Raman scattering spectroscopy with first-principles lattice dynamics calculations to reveal the charge density wave state in ScV$_6$Sn$_6$. In the low temperature phase, we find a five-fold splitting of the V-containing totally symmetric mode near 240 cm$^{-1}$ suggesting that the density wave acts to mix modes of $P$6/$mmm$ and $R$$\bar{3}$$m$ symmetry - an effect that we quantify by projecting phonons of the high symmetry state onto those of the lower symmetry structure. We also test the stability of the density wave state under compression and find that both physical and chemical pressure act to quench the effect. We discuss these findings in terms of symmetry and the structure-property trends that can be unraveled in this system.

Understanding the spin dynamics in antiferromagnetic (AFM) thin films is fundamental for designing novel devices based on AFM magnon transport. Here, we study the magnon dynamics in thin films of AFM $S=5/2$ $\alpha$-Fe$_2$O$_3$ by combining resonant inelastic x-ray scattering, Anderson impurity model plus dynamical mean-field theory, and Heisenberg spin model. Below 100 meV, we observe the thickness-independent (down to 15 nm) acoustic single-magnon mode. At higher energies (100-500 meV), an unexpected sequence of equally spaced, optical modes is resolved and ascribed to $\Delta S_z = 1$, 2, 3, 4, and 5 magnetic excitations corresponding to multiple, noninteracting magnons. Our study unveils the energy, character, and momentum-dependence of single and multimagnons in $\alpha$-Fe$_2$O$_3$ thin films, with impact on AFM magnon transport and its related phenomena. From a broader perspective, we generalize the use of L-edge resonant inelastic x-ray scattering as a multispin-excitation probe up to $\Delta S_z = 2S$. Our analysis identifies the spin-orbital mixing in the valence shell as the key element for accessing excitations beyond $\Delta S_z = 1$, and up to, e.g., $\Delta S_z = 5$. At the same time, we elucidate the novel origin of the spin excitations beyond the $\Delta S_z = 2$, emphasizing the key role played by the crystal lattice as a reservoir of angular momentum that complements the quanta carried by the absorbed and emitted photons., Comment: Accepted in Physical Review X

The manifestation of skyrmions in the Mott-insulator Cu$_2$OSeO$_3$ originates from a delicate balance between magnetic and electronic energy scales. As a result of these intertwined couplings, the two symmetry-inequivalent magnetic ions, Cu-I and Cu-II, bond into a spin S=1 entangled tetrahedron. However, conceptualizing the unconventional properties of this material and the energy of the competing interactions is a challenging task due the complexity of this system. Here we combine X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering to uncover the electronic and magnetic excitations of Cu$_2$OSeO$_3$ with site-specificity. We quantify the energies of the 3d crystal-field splitting for both Cu-I and Cu-II, fundamental to optimize model Hamiltonians. Additionally, we unveil a site-specific magnetic mode, indicating that individual spin character is preserved within the entangled-tetrahedron picture. Our results thus provide experimental constraint for validating theories that describe the interactions of Cu$_2$OSeO$_3$, highlighting the site-selective capabilities of resonant spectroscopies

Spin excitations of magnetic thin films are the founding element for novel transport concepts in spintronics, magnonics, and magnetic devices in general. While spin dynamics have been extensively studied in bulk materials, their behaviour in mesoscopic films is less known due to experimental limitations. Here, we employ Resonant Inelastic X-Ray Scattering to investigate the spin excitation spectrum in mesoscopic Fe films, from bulk-like down to 3 unit cells thick. In bulk-like samples, we find isotropic, dispersive ferromagnons consistent with the dispersion observed by neutron scattering in bulk single crystals. As the thickness is reduced, these ferromagnons survive and evolve anisotropically: renormalising to lower energies along the out-of-plane direction while retaining their dispersion in the in-plane direction. This thickness dependence is captured by simple Heisenberg model calculations accounting for the confinement in the out-of-plane direction through the loss of Fe bonds. Our findings highlight the effects of mesoscopic scaling on spin dynamics and identify thickness as a knob for fine-tuning and controlling magnetic properties in films., Comment: 17 pages, 4, figure, submitted

We report a new design of temperature-modulated dilatometer, which obtains the linear thermal expansion coefficient by measuring the oscillating changes of the sample's length and temperature by a piezobender and a thermocouple, respectively. Using an iron-based superconductor KFe$_2$As$_2$ as an example, we show that this device is able to measure thin samples with high resolutions at low temperatures and high magnetic fields. Despite its incapability of giving absolute values, the new dilatometer provides a high-resolution method to study many important physical properties in condensed matter physics, such as thermal and quantum phase transitions, and vortex dynamics in the superconducting state. The prototype design of this device can be further improved in many aspects to meet particular requirements., Comment: 6 pages, 3 figures; An error has been found in the setup and eta now can be independently determined without normalization to the standard sample

We have systematically studied the nematic susceptibility in non-superconducting Ba(Fe$_{1-x}$TM$_{x}$)$_2$As$_2$ (TM = Cr, Mn, V and Cu) by measuring the uniaxial pressure dependence of the resistivity along the Fe-As-Fe direction. The nematic susceptibilities in all samples show the Curie-Weiss-like behavior at high temperatures, where the nematic Curie constant $A_n$ can be derived, similar to the Curie constant in a paramagnetism. While all these dopants do not introduce superconductivity in BaFe$_2$As$_2$, their effects on nematic fluctuations are different. In Mn, Cr and V doped samples, $|A_n|$ decreases significantly with the increasing doping level. On the other hand, $|A_n|$ increases dramatically with Cu doping, similar to the superconducting Ni-doped BaFe$_2$As$_2$. However, the nematic susceptibility is suppressed at low temperatures for $x$ larger than $0.04$, which may be related to the short-range antiferromagnetic order that survives up to very high doping level. Doping Mn, Cr and Cu into the optimally-doped superconducting BaFe$_2$(As$_{0.69}$P$_{0.31}$)$_2$ also strongly reduces $|A_n|$. Compared with those systems that clearly exhibit superconductivity, such as Ni, K or P doped samples, our results suggest a strong connection between the nematic and spin degrees of freedom. Moreover, the reason of the suppression of superconductivity by dopants such as Cr, Mn, V and Cu may be correlated with the suppression of nematic fluctuations., Comment: 8 pages, 5 figures

We present magnetization studies as a function of time, temperature and magnetic field for $H$ $\parallel$ c-axis, in a hole-doped pnictide superconductor, La$_{0.34}$Na$_{0.66}$Fe$_2$As$_2$, with, $T_c$ $\approx$ 27 K. The obtained vortex phase-diagram shows that the magnetic irreversibility line is very close to the mean-field superconducting transition line, similar to the low $T_c$ superconductors, evidencing a strong pinning behavior. The irreversibility line does not follow a power law behavior with ($T_c$-$T$), however, it is well described using an expression developed in the literature considering the effect of disorder in the system. The critical current density estimated using the Bean's critical-state model is found to be of the order of 10$^5$ A/cm$^2$ below 12 K in the limit of zero magnetic field. A plot of the normalized pinning force density as a function of the reduced magnetic field at different temperatures shows a good scaling and the analysis suggests that the vortex pinning is due to normal point like pinning centers. The temperature dependence of the critical current density suggests that the pinning due to the variation in charge carrier mean free path alone is not sufficient to explain the experimental data. Magnetic relaxation rate as a function of temperature and magnetic field is also studied., Comment: 19 pages, 6 Figures, Accepted for Publication in the "Journal of Applied Physics 2019"

We used transport and inelastic neutron scattering to study the optimally phosphorus-doped BaFe$_2$(As$_{0.7}$P$_{0.3}$)$_2$ superconductor ($T_c = 30$ K). In the normal state, we find that the previously reported linear temperature dependence of the resistivity below room temperature extends to $\sim$ 500 K. Our analysis of the temperature and energy ($E=\hbar\omega$) dependence of spin dynamical susceptibility at the antiferromagnetic (AF) ordering wave vector $\chi^{\prime\prime}({\bf Q}_{\rm AF},\omega)$ reveal an $\omega / T$ scaling within $1.1

We report single-crystal growth of La$_{0.34}$Na$_{0.66}$Fe$_2$As$_2$ iron-based superconductor with the size of several millimeters. The samples were accidentally obtained in trying to grow LaFeAsO$_{1-y}$F$_y$ ( $y \geq$ 0.8 ) single crystals with NaAs and NaF flux. The sample shows both antiferromagnetic and structural transitions at 106 K. The superconducting transition temperature is about 27 K with the superconducting anisotropy of about 1.9. These values and the temperature dependence of the Hall coefficient suggest that La$_{0.34}$Na$_{0.66}$Fe$_2$As$_2$ belongs to hole-doped "122" families of iron pnictides with the doping level slightly lower than optimal doping. Compared with previous reports on the polycrystalline samples, our results suggest that either $T_c$ of the this system can be further increased, or the superconducting dome may not be well formed in this system. In either case, the La$_{0.5-x}$Na$_{0.5+x}$Fe$_2$As$_2$ system provides a new platform to study the antiferromagnetic and superconducting properties of iron-based superconductors., Comment: 11 pages, 5 figures

Overshadowing the superconducting dome in hole-doped cuprates, the pseudogap state is still one of the mysteries that no consensus can be achieved. It has been suggested that the rotational symmetry is broken in this state and may result in a nematic phase transition, whose temperature seems to coincide with the onset temperature of the pseudogap state $T^*$ around optimal doping level, raising the question whether the pseudogap results from the establishment of the nematic order. Here we report results of resistivity measurements under uniaxial pressure on several hole-doped cuprates, where the normalized slope of the elastoresistivity $\zeta$ can be obtained as illustrated in iron-based superconductors. The temperature dependence of $\zeta$ along particular lattice axis exhibits kink feature at $T_{k}$ and shows Curie-Weiss-like behavior above it, which may suggest a spontaneous nematic transition. While $T_{k}$ seems to be the same as $T^*$ around the optimal doping and in the overdoped region, they become very different in underdoped La$_{2-x}$Sr$_{x}$CuO$_4$. Our results suggest that the nematic order, if indeed existing, is an electronic phase within the pseudogap state., Comment: 6 pages, 4 figures

We have systematically studied the effects of in-plane uniaxial pressure $p$ on the superconducting transition temperature $T_c$ in many iron-based superconductors. The change of $T_c$ with $p$ is composed of linear and nonlinear components. The latter can be described as a quadratic term plus a much smaller fourth-order term. In contrast to the linear component, the nonlinear $p$ dependence of $T_c$ displays a pronounced in-plane anisotropy, which is similar to the anisotropic response of the resistivity to $p$. As a result, it can be attributed to the coupling between the superconducting and nematic orders, in accordance with the expectations of a phenomenological Landau theory. Our results provide direct evidences for the interplay between nematic fluctuations and superconductivity, which may be a common behavior in iron-based superconductors., Comment: 6 pages, 7 figures

Chemical substitution during growth is a well-established method to manipulate electronic states of quantum materials, and leads to rich spectra of phase diagrams in cuprate and iron-based superconductors. Here we report a novel and generic strategy to achieve nonvolatile electron doping in series of (i.e. 11 and 122 structures) Fe-based superconductors by ionic liquid gating induced protonation at room temperature. Accumulation of protons in bulk compounds induces superconductivity in the parent compounds, and enhances the Tc largely in some superconducting ones. Furthermore, the existence of proton in the lattice enables the first proton nuclear magnetic resonance (NMR) study to probe directly superconductivity. Using FeS as a model system, our NMR study reveals an emergent high-Tc phase with no coherence peak which is hard to measure by NMR with other isotopes. This novel electric-field-induced proton evolution opens up an avenue for manipulation of competing electronic states (e.g. Mott insulators), and may provide an innovative way for a broad perspective of NMR measurements with greatly enhanced detecting resolution., Comment: 11 pages, 4 figures, published, http://engine.scichina.com/publisher/scp/journal/SB/63/1/10.1016/j.scib.2017.12.009?slug=full text

We use unpolarized and polarized neutron scattering to study the temperature and polarization dependence of low-energy magnetic fluctuations in nearly-optimal-doped NaFe$_{0.9785}$Co$_{0.0215}$As, with coexisting superconductivity ($T_{\rm c}\approx19$ K) and weak antiferromagnetic order ($T_{\rm N}\approx30$ K, ordered moment $\approx0.02$ $\mu_{\rm B}$/Fe). A single spin resonance mode with intensity tracking the superconducting order parameter is observed, although energy of the mode only softens slightly on approaching $T_{\rm c}$. Polarized neutron scattering reveals that the single resonance is mostly isotropic in spin space, similar to overdoped NaFe$_{0.935}$Co$_{0.045}$As but different from optimal electron-, hole-, and isovalent-doped BaFe$_2$As$_2$ compounds, all featuring an additional prominent anisotropic component. Spin anisotropy in NaFe$_{0.9785}$Co$_{0.0215}$As is instead present at energies below the resonance, which becomes partially gapped below $T_{\rm c}$, similar to the situation in optimal-doped YBa$_2$Cu$_3$O$_{6.9}$. Our results indicate that anisotropic spin fluctuations in NaFe$_{1-x}$Co$_x$As appear in the form of a resonance in the underdoped regime, become partially gapped below $T_{\rm c}$ near optimal doping and disappear in overdoped compounds., Comment: to be published in PRB

We report a systematic crystal growth and characterization of Ca$_{1-y}$La$_{y}$Fe$_{1-x}$Ni$_{x}$As$_{2}$, the newly discovered 112-type iron-based superconductor. After substituting Fe by a small amount of Ni, bulk superconductivity is successfully obtained in high quality single crystals sized up to 6 mm. Resistivity measurements indicate common features for transport properties in this 112-type iron pnictide, suggest strong scattering from chemical dopants. Together with the superconducting transition temperature $T_c$, and the Neel temperature $T_N$ determined by the elastic neutron scattering, we sketch a three-dimensional phase diagram in the combination of both Ni and La dopings., Comment: 8 pages, 8 figures

We have systematically studied the antiferromagnetic and nematic transitions in Sr$_{1-x}$Ba$_x$Fe$_{1.97}$Ni$_{0.03}$As$_2$ by magnetic susceptibility and uniaxial-pressure resistivity measurements, respectively. The derivatives of the temperature dependence of both magnetic and nematic susceptibilities show clearly sharp peak when the transitions are first-order. Accordingly, we show that while both of the magnetic and nematic transitions change from first-order to second-order with increasing Barium doping level, there is a narrow doping range where the former becomes second-order but the latter remains first-order, which has never been realized before in other systems. Moreover, the antiferromagnetic and nematic transition temperatures become different and the jump of nematic susceptibility becomes small in this intermediate doping range. Our results provide key information on the interplay between magnetic and nematic transitions. Concerning the current debate on the microscopic models for nematicity in iron-based superconductors, these observations agree with the magnetic scenario for an itinerant fermionic model in excellent details., Comment: 5 pages, 4 figures

High-temperature superconductivity is closely adjacent to a long-range antiferromagnet, which is called a parent compound. In cuprates, all parent compounds are alike and carrier doping leads to superconductivity, so a unified phase diagram can be drawn. However, the properties of parent compounds for iron-based superconductors show significant diversity and both carrier and isovalent dopings can cause superconductivity, which casts doubt on the idea that there exists a unified phase diagram for them. Here we show that the ordered moments in a variety of iron pnictides are inversely proportional to the effective Curie constants of their nematic susceptibility. This unexpected scaling behavior suggests that the magnetic ground states of iron pnictides can be achieved by tuning the strength of nematic fluctuations. Therefore, a unified phase diagram can be established where superconductivity emerges from a hypothetical parent compound with a large ordered moment but weak nematic fluctuations, which suggests that iron-based superconductors are strongly correlated electron systems., Comment: 5 pages, 2 figures

We have systematically studied the nematic fluctuations in the electron-doped iron-based superconductor BaFe$_{2-x}$Ni$_x$As$_2$ by measuring the in-plane resistance change under uniaxial pressure. While the nematic quantum critical point can be identified through the measurements along the (110) direction as studied previously, quantum and thermal critical fluctuations cannot be distinguished due to similar Curie-Weiss-like behaviors. Here we find that a sizable pressure-dependent resistivity along the (100) direction is present in all doping levels, which is against the simple picture of an Ising-type nematic model. The signal along the (100) direction becomes maximum at optimal doping, suggesting that it is associated with nematic quantum critical fluctuations. Our results indicate that thermal fluctuations from striped antiferromagnetic order dominate the underdoped regime along the (110) direction. We argue that either there is a strong coupling between the quantum critical fluctuations and the fermions, or more exotically, a higher symmetry may be present around optimal doping., Comment: 5 pages, 3 figures. This Letter only contains parts of the former version 1511.05784