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Antiferromagnetically coupled S=1/2 spins on an isotropic triangular lattice is the paradigm of frustrated quantum magnetism, but structurally ideal realizations are rare. Here we investigate NaYbO2, which hosts an ideal triangular lattice of Jeff=1/2 moments with no inherent site disorder. No signatures of conventional magnetic order appear down to 50 mK, strongly suggesting a quantum spin liquid ground state. We observe a two-peak specific heat and a nearly quadratic temperature dependence in accord with expectations for a two-dimensional Dirac spin liquid. Application of a magnetic field strongly perturbs the quantum disordered ground state and induces a clear transition into a collinear ordered state consistent with a long-predicted "up-up-down" structure for a triangular lattice XXZ Hamiltonian driven by quantum fluctuations. The observation of spin liquid signatures in zero field and quantum-induced ordering in intermediate fields in the same compound demonstrate an intrinsically quantum disordered ground state. We conclude that NaYbO2 is a model, versatile platform for exploring spin liquid physics with full tunability of field and temperature.Exotic ground states of quantum antiferromagnets are encouraged by the combination of low dimensionality, geometric frustration, and inherent anisotropies. Planar triangular lattices have long been sought as platforms for stabilizing them 1-7 ; however, ideal manifestations that do not break crystallographic or exchange symmetries upon approaching the quantum regime are rare. The organic compounds κ-(BEDT-TTF)2Cu2(CN)3 8 and EtMe3Sb[Pd(dmit)2]2 9 are two promising examples of triangular lattices with S=1/2 moments and a dynamically disordered spin ground state. However, S=1/2 inorganic analogs such as Ba3CoSb2O9 10 , Ba8CoNb6O24 11 , and NaTiO2 12-14 either order magnetically or undergo a lattice deformation and dimerization upon cooling. A key roadblock in inorganic systems is the identification of a material with a high crystallographic symmetry, rigid structure, and minimal defect mechanisms that also contains magnetic ions possessing strong quantum fluctuations. Ideally, the magnetic ions should be located at high symmetry positions that preclude antisymmetric Dzyaloshinskii-Moriya exchange from lifting geometric frustration at low temperatures.As an alternative to S=1/2 based compounds, rare earth ions with ground state doublets may also engender enhanced quantum fluctuations when decorating a triangular lattice. Specifically, recent studies have shown that the spin-orbit entangled Jeff=1/2 moments of Yb 3+ ions on this lattice may exhibit a variety of nearly degenerate magnetic states 15-22 . Given the appropriate anisotropies and when driven close

Exploration of spin currents in organic semiconductors (OSECs) induced by resonant microwave absorption in ferromagnetic substrates is appealing for potential spintronics applications. Owing to the inherently weak spin-orbit coupling (SOC) of OSECs, their inverse spin Hall effect (ISHE) response is very subtle; limited by the microwave power applicable under continuous-wave (cw) excitation. Here we introduce a novel approach for generating significant ISHE signals in OSECs using pulsed ferromagnetic resonance, where the ISHE is two to three orders of magnitude larger compared to cw excitation. This strong ISHE enables us to investigate a variety of OSECs ranging from π-conjugated polymers with strong SOC that contain intrachain platinum atoms, to weak SOC polymers, to C60 films, where the SOC is predominantly caused by the curvature of the molecule's surface. The pulsed-ISHE technique offers a robust route for efficient injection and detection schemes of spin currents at room temperature, and paves the way for spin orbitronics in plastic materials.

The effects of external magnetic fields on the electrical conductivity of organic semiconductors have been attributed to hyperfine coupling of the spins of the charge carriers and hydrogen nuclei. We studied this coupling directly by implementation of pulsed electrically detected nuclear magnetic resonance spectroscopy in organic light-emitting diodes (OLEDs). The data revealed a fingerprint of the isotope (protium or deuterium) involved in the coherent spin precession observed in spin-echo envelope modulation. Furthermore, resonant control of the electric current by nuclear spin orientation was achieved with radiofrequency pulses in a double-resonance scheme, implying current control on energy scales one-millionth the magnitude of the thermal energy.

Pairs of charge-carrier spins in organic semiconductors constitute four-level systems that can be driven electromagnetically 1 . Given appropriate conditions for ultrastrong coupling 2 -weak local hyperfine fields B hyp , large magnetic resonant driving fields B 1 and low static fields B 0 that define Zeeman splittingthe spin-Dicke e ect, a collective transition of spin states, has been predicted 3 . This parameter range is challenging to probe by electron paramagnetic resonance spectroscopy because thermal magnetic polarization is negligible. It is accessed through spin-dependent conductivity that is controlled by electron-hole pairs of singlet and triplet spin-permutation symmetry without the need of thermal spin polarization 4 . Signatures of collective behaviour of carrier spins are revealed in the steady-state magnetoresistance of organic light-emitting diodes (OLEDs), rather than through radiative transitions. For intermediate B 1 , the a.c.-Zeeman e ect appears. For large B 1 , a collective spin-ensemble state arises, inverting the current change under resonance and removing power broadening, thereby o ering a unique window to ambient macroscopic quantum coherence.Macroscopic phase coherence is a hallmark of many exotic states of matter such as superconductivity, ferromagnetism or BoseEinstein condensation. Such coherence may also emerge between two-level systems, where it is mediated by electromagnetic fields, as described by the Dicke effect in collisional narrowing 5 and superradiance 6 . Collective behaviour may already arise within a pair of interacting two-level systems 7 , an observation that can potentially be extended to the prototypical two-level system of an electron spin. For pairs of charge-carrier spins in organic semiconductors, with driving fields B 1 exceeding the hydrogen-induced random local hyperfine field 1 B hyp and approaching the magnitude of the static magnetic field B 0 , a collective macroscopic spin phase has been predicted to emerge 3 . Under these conditions, when the spin-Rabi splitting becomes comparable to the Zeeman splitting, the electromagnetic field links individually resonant spin pairs together, forming a spin-Dicke state analogous to that in the dipolar Dicke effect [5][6][7] . These macroscopic effects are observable through measurements of electronic recombination rates, which depend on spin-permutation symmetry of the pair 8 .We monitor the electron-hole recombination current in an OLED, where positive and negative charges are injected into a thin film of an organic semiconductor from opposite electrodes. As the charges drift through the material, they can capture each other on intermolecular length scales owing to weak dielectric screening. These weakly coupled intermolecular electron-hole pairs 9 can ultimately recombine on individual molecules to form a molecular excited state, or exciton, which gives rise to electroluminescence. The subsequent discussion focuses on carrier pairs and not on excitons, which have spin S = 0 or 1. Because the carriers possess spi...

Separating the influence of hyperfine from spin-orbit interactions in spin-dependent carrier recombination and dissociation processes necessitates magnetic resonance spectroscopy over a wide range of frequencies.We have designed compact and versatile coplanar waveguide resonators for continuous-wave electrically detected magnetic resonance, and tested these on organic light-emitting diodes. By exploiting both the fundamental and higher-harmonic modes of the resonators we cover almost five octaves in resonance frequency within a single setup. The measurements with a common π-conjugated polymer as the active material reveal small but non-negligible effects of spin-orbit interactions, which give rise to a broadening of the magnetic resonance spectrum with increasing frequency. a)

Magnonics concepts utilize spin-wave quanta (magnons) for information transmission, processing and storage. To convert information carried by magnons into an electric signal promises compatibility of magnonic devices with conventional electronic devices, that is, magnon spintronics . Magnons in inorganic materials have been studied widely with respect to their generation, transport and detection . In contrast, resonant spin waves in the room-temperature organic-based ferrimagnet vanadium tetracyanoethylene (V(TCNE) (x ≈ 2)), were detected only recently . Herein we report room-temperature coherent magnon generation, transport and detection in films and devices based on V(TCNE) using three different techniques, which include broadband ferromagnetic resonance (FMR), Brillouin light scattering (BLS) and spin pumping into a Pt adjacent layer. V(TCNE) can be grown as neat films on a large variety of substrates, and it exhibits extremely low Gilbert damping comparable to that in yttrium iron garnet. Our studies establish an alternative use for organic-based magnets, which, because of their synthetic versatility, may substantially enrich the field of magnon spintronics.

Spin-dependent processes play a crucial role in organic electronic devices. Spin coherence can give rise to spin mixing due to a number of processes such as hyperfine coupling, and leads to a range of magnetic field effects. However, it is not straightforward to differentiate between pure single-carrier spin-dependent transport processes which control the current and therefore the electroluminescence, and spin-dependent electron-hole recombination which determines the electroluminescence yield and in turn modulates the current. We therefore investigate the correlation between the dynamics of spin-dependent electric current and spin-dependent electroluminescence in two derivatives of the conjugated polymer poly(phenylene-vinylene) using simultaneously measured pulsed electrically detected (pEDMR) and optically detected (pODMR) magnetic resonance spectroscopy. This experimental approach requires careful analysis of the transient response functions under optical and electrical detection. At room temperature and under bipolar charge-carrier injection conditions, a correlation of the pEDMR and the pODMR signals is observed, consistent with the hypothesis that the recombination currents involve spin-dependent electronic transitions. This observation is inconsistent with the hypothesis that these signals are caused by spin-dependent charge carrier transport. These results therefore provide no evidence that supports earlier claims that spindependent transport plays a role for room temperature magnetoresistance effects. At low temperatures, however, the correlation between pEDMR and pODMR is weakened, demonstrating that more than one spin-dependent process influences the optoelectronic materials properties. This conclusion is consistent with prior studies of half-field resonances that were attributed to spin-dependent triplet exciton recombination which becomes significant at low temperatures when the triplet lifetime increases. PACS