arXiv subjects

L. Forró

Publications and source records attributed to L. Forró.

At least 19 recordsLinked to original sources

arXiv2026

Telecom-Wavelength-Compatible Quantum Information Transcription Using Nitrogen-Vacancy Centers

Nitrogen-vacancy (NV) centers in diamond are a leading platform for solid-state quantum sensing and quantum information processing. While most optical studies rely on the visible fluorescence associated with the triplet transitions, the infrared singlet transition near $1042$ nm, which is typically considered dark within the singlet manifold of the NV optical cycle, provides an alternative optical channel. Here, we report wavelength-resolved optically detected magnetic resonance (ODMR) measurements of this infrared emission. We directly observe ODMR contrast in the $1042$ nm emission and analyze its dependence on the magnetic field. The field-dependent spectral dispersion of the ODMR signal demonstrates that the spin-state information encoded in the NV center is transcribed to the infrared singlet emission through the spin-selective intersystem crossing, in close analogy to the visible fluorescence readout. These results establish infrared ODMR as a high-fidelity optical readout pathway. Crucially, by extending spin-state transcription directly into the $1300-1600$ nm range, this work demonstrates a direct, conversion-free interface between diamond spin-qubits and standard telecommunication infrastructure, bypassing the efficiency bottlenecks of active frequency conversion and benefiting from the already well-developed technologies in this range of the electromagnetic spectrum.

cond-mat.mtrl-sci↗

arXiv2024

High-entropy magnetism of murunskite

Murunskite (K$_2$FeCu$_3$S$_4$) is a bridging compound between the only two known families of high-temperature superconductors. It is a semiconductor like the parent compounds of cuprates, yet isostructural to metallic iron-pnictides. Moreover, like both families, it has an antiferromagnetic (AF)-like response with an ordered phase occurring below $\approx$ 100 K. Through comprehensive neutron, Mössbauer, and XPS measurements on single crystals, we unveil AF with a nearly commensurate quarter-zone wave vector. Intriguingly, the only identifiable magnetic atoms, iron, are randomly distributed over one-quarter of available crystallographic sites in 2D planes, while the remaining sites are occupied by closed-shell copper. Notably, any interpretation in terms of a spin-density wave is challenging, in contrast to the metallic iron-pnictides where Fermi-surface nesting can occur. Our findings align with a disordered-alloy picture featuring magnetic interactions up to second neighbors. Moreover, in the paramagnetic state, iron ions are either in Fe$^{3+}$ or Fe$^{2+}$ oxidation states, associated with two distinct paramagnetic sites identified by Mössbauer spectroscopy. Upon decreasing the temperature below the appearance of magnetic interactions, these two signals merge completely into a third, implying an orbital transition. It completes the cascade of (local) transitions that transform iron atoms from fully orbitally and magnetically disordered to homogeneously ordered in inverse space, but still randomly distributed in real space.

cond-mat.str-el↗

arXiv2023

Beyond 1 ms Charge-Carrier Recombination Dynamics in the CsPbBr3 Perovskite

Knowledge of the charge-carrier recombination lifetime, tau, is crucial for the various applications of photovoltaic perovskites. We studied the novel inorganic perovskite, CsPbBr3 and we observe recombination dynamics beyond 1 ms below 200 K and tau approaching 100 us at room temperature. Time-resolved microwave-detected photoconductivity decay (TRMCD), used in combination with injection dependence, evidence that tau is dominated by impurity charge trapping. The observed injection dependence is well corroborated by modeling of the trap mechanism. The ultra-long decay time is also consistent with photoconductivity measurements with a continuous-wave excitation at powers corresponding to around one Sun irradiation. While in principle charge-carrier trapping may limit the photovoltaic efficiency in single-cell photovoltaic devices, it could also lead to enhanced efficiency in tandem cells as well as for alternative applications including photodetection and quantum information storage.

physics.app-ph↗

arXiv2023

Ultralong 100 ns Spin Relaxation Time in Graphite at Room Temperature

Graphite has been intensively studied, yet its electron spins dynamics remains an unresolved problem even 70 years after the first experiments. The central quantities, the longitudinal ($T_1$) and transverse ($T_2$) relaxation times were postulated to be equal, mirroring standard metals, but $T_1$ has never been measured for graphite. Here, based on a detailed band structure calculation including spin-orbit coupling, we predict an unexpected behavior of the relaxation times. We find, based on saturation ESR measurements, that $T_1$ is markedly different from $T_2$. Spins injected with perpendicular polarization with respect to the graphene plane have an extraordinarily long lifetime of $100$ ns at room temperature. This is ten times more than in the best graphene samples. The spin diffusion length across graphite planes is thus expected to be ultralong, on the scale of $\sim 70~μ$m, suggesting that thin films of graphite -- or multilayer AB graphene stacks -- can be excellent platforms for spintronics applications compatible with 2D van der Waals technologies. Finally, we provide a qualitative account of the observed spin relaxation based on the anisotropic spin admixture of the Bloch states in graphite obtained from density functional theory calculations.

cond-mat.mes-hall↗

arXiv2023

Uncertainties in experiments on strongly-coupled vacuum field modification of superconductivity and ferromagnetism in solids

We discuss recent experiments in which fine particles of the organic superconductor Rb$_3$C$_{60}$ or the cuprate superconductor YBa$_2$Cu$_3$O$_{6+x}$ are held in a polystyrene film that is spin-coated on to a silicon substrate with or without an intervening gold, or another inert metallic layer. From SQUID magnetisation data for Rb$_3$C$_{60}$ there appears to be a striking and completely unexpected increase in the superconducting transition temperature from $30$ to $45$~K, which is ascribed to coupling between the electrons in the superconductor and vacuum fluctuations in the electromagnetic field just above the metallic film. We argue that this could be a non-intrinsic effect associated with the presence of solid oxygen in the Pyrex sample tube. We suggest that the ferromagnetic SQUID signal observed for YBa$_2$Cu$_3$O$_{6+x}$ particles in polystyrene could be attributed to ferromagnetic particles or magnetic clusters of unknown origin.

cond-mat.supr-con↗

arXiv2021

Ultrahigh nitrogen-vacancy center concentration in diamond

High concentration of negatively charged nitrogen-vacancy ($\text{NV}^{-}$) centers was created in diamond single crystals containing approximately 100 ppm nitrogen using electron and neutron irradiation and subsequent thermal annealing in a stepwise manner. Continuous wave electron paramagnetic resonance (EPR) was used to determine the transformation efficiency from isolated N atoms to $\text{NV}^{-}$ centers in each production step and its highest value was as high as 17.5 %. Charged vacancies are formed after electron irradiation as shown by EPR spectra, but the thermal annealing restores the sample quality as the defect signal diminishes. We find that about 25 % of the vacancies form NVs during the annealing process. The large $\text{NV}^{-}$ concentration allows to observe orientation dependent spin-relaxation times and also the determination of the hyperfine and quadrupole coupling constants with high precision using electron spin echo (ESE) and electron-nuclear double resonance (ENDOR). We also observed the EPR signal associated with the so-called W16 centers, whose spectroscopic properties might imply a nitrogen dimer-vacancy center for its origin.

cond-mat.mtrl-sci↗

arXiv2020

Tuning Conductivity and Spin Dynamics in Few-Layer Graphene via In Situ Potassium Exposure

Chemical modification, such as intercalation or doping of novel materials is of great importance for exploratory material science and applications in various fields of physics and chemistry. In the present work, we report the systematic intercalation of chemically exfoliated few-layer graphene with potassium while monitoring the sample resistance using microwave conductivity. We find that the conductivity of the samples increases by about an order of magnitude upon potassium exposure. The increased of number of charge carriers deduced from the ESR intensity also reflects this increment. The doped phases exhibit two asymmetric Dysonian lines in ESR, a usual sign of the presence of mobile charge carriers. The width of the broader component increases with the doping steps, however, the narrow components seem to have a constant line width.

cond-mat.mtrl-sci↗

arXiv2020

Ultralong spin lifetime in light alkali atom doped graphene

Today's great challenges of energy and informational technologies are addressed with a singular compound, the Li and Na doped few layer graphene. All what is impossible for graphite (homogeneous and high level Na doping), and unstable for single layer graphene, works very well for this structure. The transformation of the Raman G line to a Fano lineshape and the emergence of strong, metallic-like electron spin resonance (ESR) modes, attest the high level of graphene doping in liquid ammonia for both kinds of alkali atoms. The spin-relaxation time in our materials, deduced from the ESR line-width, is 6-8 ns, which is comparable to the longest values found in spin-transport experiments on ultrahigh mobility graphene flakes. This could qualify our material as promising candidate in spintronics devices. On the other hand, the successful sodium doping, this being a highly abundant metal, could be an encouraging alternative to lithium batteries.

cond-mat.mtrl-sci↗

arXiv2019

Improved alkali intercalation of carbonaceous materials in ammonia solution

Alkali intercalated graphite compounds represent a compelling modification of carbon with significant application potential and various fundamentally important phases. We report on the intercalation of graphite with alkali atoms (Li and K) using liquid ammonia solution as mediating agent. Alkali atoms dissolve well in liquid ammonia which simplifies and speeds up the intercalation process, and it also avoids the high temperature formation of alkali carbides. Optical microscopy, Raman, and electron spin resonance spectroscopy attest that the prepared samples are highly and homogeneously intercalated to a level approaching Stage-I intercalation compounds. The method and the synthesis route may serve as a starting point for the various forms of alkali atom intercalated carbon compounds (including carbon nanotubes and graphene), which could be exploited in energy storage and further chemical modifications.

cond-mat.str-el↗

arXiv2019

Incidence of multilayers in chemically exfoliated graphene

An efficient route to synthesize macroscopic amounts of graphene is highly desired and a bulk characterization of such samples, in terms of the number of layers, is equally important. We present a Raman spectroscopy-based method to determine the distribution of the number of graphene layers in chemically exfoliated graphene. We utilize a controlled vapor-phase potassium intercalation technique and identify a lightly doped stage, where the Raman modes of undoped and doped few-layer graphene flakes coexist. The spectra can be unambiguously distinguished from alkali doped graphite, and a modeling with the distribution of the layers yields an upper limit of flake thickness of five layers with a significant single-layer graphene content. Complementary statistical AFM measurements on individual few-layer graphene flakes find a consistent distribution of the layer numbers.

cond-mat.mes-hall↗

arXiv2017

Charge-Stripe Order and Superconductivity in $\mathrm{Ir_{1-x}Pt_xTe_2}$

A combined resistivity and hard x-ray diffraction study of superconductivity and charge ordering in $\mathrm{Ir_{1-x}Pt_xTe_2}$, as a function of Pt substitution and externally applied hydrostatic pressure, is presented. Experiments are focused on samples near the critical composition $x_c\sim 0.045$ where competition and switching between charge order and superconductivity is established. We show that charge order as a function of pressure in $\mathrm{Ir_{0.95}Pt_{0.05}Te_{2}}$ is preempted - and hence triggered - by a structural transition. Charge ordering appears uniaxially along the short crystallographic (1,0,1) domain axis with a $\mathrm{(\frac{1}{5},0,\frac{1}{5})}$ modulation. Based on these results we draw a charge-order phase diagram and discuss the relation between stripe ordering and superconductivity.

cond-mat.supr-con↗

arXiv2017

$J_1$-$J_2$ square lattice antiferromagnetism in the orbitally quenched insulator MoOPO$_4$

We report magnetic and thermodynamic properties of a $4d^1$ (Mo$^{5+}$) magnetic insulator MoOPO$_4$ single crystal, which realizes a $J_1$-$J_2$ Heisenberg spin-$1/2$ model on a stacked square lattice. The specific-heat measurements show a magnetic transition at 16 K which is also confirmed by magnetic susceptibility, ESR, and neutron diffraction measurements. Magnetic entropy deduced from the specific heat corresponds to a two-level degree of freedom per Mo$^{5+}$ ion, and the effective moment from the susceptibility corresponds to the spin-only value. Using {\it ab initio} quantum chemistry calculations we demonstrate that the Mo$^{5+}$ ion hosts a purely spin-$1/2$ magnetic moment, indicating negligible effects of spin-orbit interaction. The quenched orbital moments originate from the large displacement of Mo ions inside the MoO$_6$ octahedra along the apical direction. The ground state is shown by neutron diffraction to support a collinear Néel-type magnetic order, and a spin-flop transition is observed around an applied magnetic field of 3.5 T. The magnetic phase diagram is reproduced by a mean-field calculation assuming a small easy-axis anisotropy in the exchange interactions. Our results suggest $4d$ molybdates as an alternative playground to search for model quantum magnets.

cond-mat.str-el↗

arXiv2016

Magnetotransport studies of Superconducting Pr$_4$Fe$_2$As$_2$Te$_{1-x}$O$_4$

We report a detailed study of the electrical transport properties of single crystals of Pr$_4$Fe$_2$As$_2$Te$_{1-x}$O$_4$, a recently discovered iron-based superconductor. Resistivity, Hall effect and magnetoresistance are measured in a broad temperature range revealing the role of electrons as dominant charge carriers. The significant temperature dependence of the Hall coefficient and the violation of Kohler's law indicate multiband effects in this compound. The upper critical field and the magnetic anisotropy are investigated in fields up to 16 T, applied parallel and perpendicular to the crystallographic c-axis. Hydrostatic pressure up to 2 GPa linearly increases the critical temperature and the resistivity residual ratio. A simple two-band model is used to describe the transport and magnetic properties of Pr$_4$Fe$_2$As$_2$Te$_{1-x}$O$_4$. The model can successfully explain the strongly temperature dependent negative Hall coefficient and the high magnetic anisotropy assuming that the mobility of electrons is higher than that of holes.

cond-mat.supr-con↗

arXiv2016

Micro-engineered CH$_3$NH$_3$PbI$_3$ nanowire/graphene phototransistor for low intensity light detection at room temperature

Methylammonium lead iodide perovskite has revolutionized the field of third generation solid-state solar cells leading to simple solar cell structures1 and certified efficiencies up to 20.1%. Recently the peculiar light harvesting properties of organometal halide perovskites have been exploited in photodetectors where responsivities of ~3.5 A/W and 180 A/W have been respectively achieved for pure perovskite-based devices and hybrid nanostructures. Here, we report on the first hybrid phototransistors where the performance of a network of photoactive Methylammonium Lead Iodide nanowires (hereafter MAPbI$_3$NW) are enhanced by CVD-grown monolayer graphene. These devices show responsivities as high as ~2.6x10$^6$ A/W in the visible range showing potential as room-temperature single-electron detector.

cond-mat.mes-hall↗

arXiv2016

Ultrasensitive 1D field-effect phototransistor: CH$_3$NH$_3$PbI$_3$ nanowire sensitized individual carbon nanotube

Field-effect phototransistors were fabricated based on individual carbon nanotubes (CNTs) sensitized by CH$_3$NH$_3$PbI$_3$ nanowires (MAPbI$_3$NW). These devices represent light responsivities of R=7.7x10$^5$ A/W at low-lighting conditions in the nWmm$^{-2}$ range, unprecedented among CNT-based photo detectors. At high incident power (~1 mWmm$^{-2}$), light soaking results in a negative photocurrent, the device turns insulating. We interpret the phenomenon as a result of efficient electron-hole separation and charge transfer of holes from the perovskite to the carbon nanotube, which improves conductance by increasing the number of carriers, but leaves electrons behind. At high illumination intensity the random electrostatic potential of these quench the mobility in the nanotube. The single CNT device geometry allows the local study of the MAPbI$_3$NW/CNT interface for metallic and semiconducting CNTs separately. Infrared and Raman spectroscopy studies of CNT-CH$_3$NH$_3$PbI$_3$ composites revealed that photo-doping takes place at the interface.

cond-mat.mes-hall↗

arXiv2016

Optically switched magnetism in photovoltaic perovskite CH$_3$NH$_3$(Mn:Pb)I$_3$

The demand for ever-increasing density of information storage and speed of manipulation boosts an intense search for new magnetic materials and novel ways of controlling the magnetic bit. Here, we report the synthesis of a ferromagnetic photovoltaic CH$_3$NH$_3$(Mn:Pb)I$_3$ material in which the photo-excited electrons rapidly melt the local magnetic order through the Ruderman-Kittel-Kasuya-Yosida interactions without heating up the spin system. Our finding offers an alternative, very simple and efficient way of optical spin control, and opens an avenue for applications in low power, light controlling magnetic devices.

cond-mat.mtrl-sci↗

arXiv2016

Frustration induced one-dimensionality in the isosceles triangular antiferromagnetic lattice of $δ$-(EDT-TTF-CONMe$_{2}$)$_{2}$AsF$_6$

The $1/4$-filled organic compound, $δ$-(EDT-TTF-CONMe$_{2}$)$_{2}$AsF$_6$ is a frustrated two-dimensional triangular magnetic system as shown by high-frequency (111.2 and 222.4 GHz) electron spin resonance (ESR) and structural data in the literature. The material gradually orders antiferromagnetically below 40~K but some magnetically disordered domains persist down to 4 K. We propose that in defect free regions frustration prevents true magnetic order down to at least 4 K in spite of the large first- and second-neighbor exchange interactions along chains and between chains, respectively. The antiferromagnetic (AFM) order gradually developing below 40 K nucleates around structural defects that locally cancel frustration. Two antiferromagnetic resonance modes mapped in the principal planes at 4~K are assigned to the very weakly interacting one-dimensional molecular chains in antiferromagnetic regions.

cond-mat.str-el↗

arXiv2016

Possibility of an unconventional spin state of Ir$^{4+}$ in Ba$_{21}$Ir$_9$O$_{43}$ single crystal

We report the synthesis of single crystals of a novel layered iridate Ba$_{21}$Ir$_9$O$_{43}$, and present the crystallographic, transport and magnetic properties of this material. The compound has a hexagonal structure with two iridium oxide layers stacked along the $c$ direction. One layer consists of a triangular arrangement of Ir$_2$O$_9$ dimers while the other layer comprises two regular octahedra and one triangular pyramid, forming inter-penetrated triangular lattices. The resistivity as a function of temperature exhibits an insulating behavior, with a peculiar $T^{-3}$ behavior. Magnetic susceptibility shows antiferromagnetic Curie-Weiss behavior with $Θ_\mathrm{CW} \simeq -$90 K while a magnetic transition occurs at substantially lower temperature of 9 K. We discuss possible valence states and effective magnetic moments on Ir ions in different local environments, and argue that the Ir ions in a unique triangular-pyramidal configuration likely carry unusually large magnetic moments.

cond-mat.str-el↗