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B. G. Márkus

Publications and source records attributed to B. G. Márkus.

At least 19 recordsLinked to original sources

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↗

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↗

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↗

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↗

Optical-microwave pump-probe studies of electronic properties in novel materials

Combined microwave-optical pump-probe methods are emerging to study the quantum state of spin qubit centers and the charge dynamics in semiconductors. A major hindrance is the limited bandwidth of microwave irradiation/detection circuitry which could be overcome with the use of broadband coplanar waveguides (CPW). We present the development and performance characterization of two spectrometers: an optically detected magnetic resonance spectrometer (ODMR) and a microwave detected photoconductivity measurement. In the first method light serves as detection and microwaves excite the investigated medium, while in the second the roles are interchanged. The performance is demonstrated by measuring ODMR maps on the nitrogen-vacancy center in diamond and time resolved photoconductivity in p-doped silicon. The results demonstrate both an efficient coupling of the microwave irradiation to the samples as well as an excellent sensitivity for minute changes in sample conductivity.

physics.app-ph↗

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↗

Ultrafast sensing of photoconductivity decay using microwave resonators

Microwave reflectance probed photoconductivity (or $μ$-PCD) measurement represents a contactless and non-invasive method to characterize impurity content in semiconductors. Major drawbacks of the method include a difficult separation of reflectance due to dielectric and conduction effects and that the $μ$-PCD signal is prohibitively weak for highly conducting samples. Both of these limitations could be tackled with the use of microwave resonators due to the well-known sensitivity of resonator parameters to minute changes in the material properties combined with a null measurement. A general misconception is that time resolution of resonator measurements is limited beyond their bandwidth by the readout electronics response time. While it is true for conventional resonator measurements, such as those employing a frequency sweep, we present a time-resolved resonator parameter readout method which overcomes these limitations and allows measurement of complex material parameters and to enhance $μ$-PCD signals with the ultimate time resolution limit being the resonator time constant. This is achieved by detecting the transient response of microwave resonators on the timescale of a few 100 ns \emph{during} the $μ$-PCD decay signal. The method employs a high-stability oscillator working with a fixed frequency which results in a stable and highly accurate measurement.

physics.app-ph↗

Improved laser based photoluminescence on single-walled carbon nanotubes

Photoluminescence (PL) has become a common tool to characterize various properties of single-walled carbon nanotube (SWCNT) chirality distribution and the level of tube individualization in SWCNT samples. Most PL studies employ conventional lamp light sources whose spectral distribution is filtered with a monochromator but this results in a still impure spectrum with a low spectral intensity. Tunable dye lasers offer a tunable light source which cover the desired excitation wavelength range with a high spectral intensity, but their operation is often cumbersome. Here, we present the design and properties of an improved dye-laser system which is based on a Q-switch pump laser. The high peak power of the pump provides an essentially threshold-free lasing of the dye laser which substantially improves the operability. It allows operation with laser dyes such as Rhodamin 110 and Pyridin 1, which are otherwise on the border of operation of our laser. Our system allows to cover the 540-730 nm wavelength range with 4 dyes. In addition, the dye laser output pulses closely follow the properties of the pump this it directly provides a time resolved and tunable laser source. We demonstrate the performance of the system by measuring the photoluminescence map of a HiPco single-walled carbon nanotubes sample.

physics.app-ph↗

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↗

A highly accurate determination of absorbed power during nanomagnetic hyperthermia

Absorbed power of nanoparticles during magnetic hyperthermia can be well determined from changes in the quality factor ($Q$ factor) of a resonator, in which the radiofrequency (RF) absorbent is placed. We present an order of magnitude improvement in the $Q$ factor measurement accuracy over conventional methods by studying the switch-on and off transient signals of the resonators. A nuclear magnetic resonance (NMR) console is ideally suited to acquire the transient signals and it also allows to employ the so-called pulse phase-cycling to remove transient artifacts. The improved determination of the absorbed power is demonstrated on various resonators in the 1-30 MHz range including standard solenoids and also a birdcage resonator. This leads to the possibility to detect minute amounts of ferrite nanoparticles which are embedded in the body and also the amount of the absorbed power. We demonstrate this capability on a phantom study, where the exact location of an embedded ferrite is clearly detected.

physics.app-ph↗

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↗

Electronic properties of air-sensitive nanomaterials probed with microwave impedance measurements

Characterization of electronic properties of novel materials is of great importance for exploratory materials development and also for the discovery of new correlated phases. As several novel compounds are available in powder form only, contactless methods, which also work on air sensitive samples, are higly desired. We present that the microwave cavity perturbation technique is a versatile tool to study conductivity in such systems. The examples include studies on semiconducting-metallic crossover in carbon nanotubes upon alkali doping, study of vortex motion in the K$_3$C$_{60}$ superconductor, and the characterization of various alkali atom doped phases of black phosphorus.

physics.app-ph↗

A highly accurate measurement of resonator $Q$-factor and resonance frequency

The microwave cavity perturbation method is often used to determine material parameters (electric permittivity and magnetic permeability) at high frequencies and it relies on measurement of the resonator parameters. We present a method to determine the $Q$-factor and resonance frequency of microwave resonators which is conceptually simple but provides a sensitivity for these parameters which overcomes those of existing methods by an order of magnitude. The microwave resonator is placed in a feedback resonator setup, where the output of an amplifier is connected to its own input with the resonator as a band pass filter. After reaching steady-state oscillation, the feedback circuit is disrupted by a fast microwave switch and the transient signal, which emanates from the resonator, is detected using down-conversion. The Fourier transform of the resulting time-dependent signal yields directly the resonance profile of the resonator. Albeit the method is highly accurate, this comes with a conceptual simplicity, ease of implementation and lower circuit cost. We compare existing methods for this type of measurement to explain the sensitivity of the present technique and we also make a prediction for the ultimate sensitivity for the resonator $Q$ and $f_0$ determination.

physics.app-ph↗

Giant microwave absorption in fine powders of superconductors

Enhanced microwave absorption, larger than that in the normal state, is observed in fine grains of type-II superconductors (MgB$_2$ and K$_3$C$_{60}$) for magnetic fields as small as a few $\%$ of the upper critical field. The effect is predicted by the theory of vortex motion in type-II superconductors, however its direct observation has been elusive due to skin-depth limitations; conventional microwave absorption studies employ larger samples where the microwave magnetic field exclusion significantly lowers the absorption. We show that the enhancement is observable in grains smaller than the penetration depth. A quantitative analysis on K$_3$C$_{60}$ in the framework of the Coffey--Clem (CC) theory explains well the temperature dependence of the microwave absorption and also allows to determine the vortex pinning force constant.

cond-mat.supr-con↗

Non-calorimetric determination of absorbed power during magnetic nanoparticle based hyperthermia

Nanomagnetic hyperthermia (NMH) is intensively studied with the prospect of cancer therapy. A major challenge is to determine the dissipated power during in vivo conditions and conventional methods are either invasive or inaccurate. We present a non-calorimetric method which yields the heat absorbed during hyperthermia: it is based on accurately measuring the quality factor change of a resonant radio frequency circuit which is employed for the irradiation. The approach provides the absorbed power in real-time, without the need to monitor the sample temperature as a function of time. As such, it is free from the problems caused by the non-adiabatic heating conditions of the usual calorimetry. We validate the method by comparing the dissipated power with a conventional calorimetric measurement. We present the validation for two types of resonators with very different filling factors: a solenoid and a so-called birdcage coil. The latter is a volume coil, which is generally used in magnetic resonance imaging (MRI) under in vivo condition. The presented method therefore allows to effectively combine MRI and thermotherapy and is thus readily adaptable to existing imaging hardware.

physics.med-ph↗

Heating causes non-linear microwave absorption anomaly in single wall carbon nanotubes

Microwave impedance measurements indicate a non-linear absorption anomaly in single wall carbon nanotubes at low temperatures (below $20$ K). We investigate the nature of the anomaly using a time resolved microwave impedance measurement technique. It proves that the anomaly has an extremely slow, a few hundred second long dynamics. This strongly suggests that the anomaly is not caused by an intrinsic electronic effect and that it is rather due to a slow heat exchange between the sample and the environment.

cond-mat.mes-hall↗

Doped carbon nanotubes as a model system of biased graphene

Albeit difficult to access experimentally, the density of states (DOS) is a key parameter in solid state systems which governs several important phenomena including transport, magnetism, thermal, and thermoelectric properties. We study DOS in an ensemble of potassium intercalated single-wall carbon nanotubes (SWCNT) and show using electron spin resonance spectroscopy that a sizeable number of electron states are present, which gives rise to a Fermi-liquid behavior in this material. A comparison between theoretical and the experimental DOS indicates that it does not display significant correlation effects, even though the pristine nanotube material shows a Luttinger-liquid behavior. We argue that the carbon nanotube ensemble essentially maps out the whole Brillouin zone of graphene thus it acts as a model system of biased graphene.

cond-mat.str-el↗

Electronic and ionic conductivities in superionic Li$_4$C$_{60}$

The $10$ GHz microwave conductivity, $σ(T)$ and high field, $222$ GHz electron spin resonance (HF-ESR) of Li$_4$C$_{60}$ fulleride is measured in a wide temperature range. We suggest that the majority of ESR active sites and at least some of the charge carriers for $σ(T)$ are electrons bound to a small concentration of surplus or vacancy ions in the polymer phase. Both $σ(T)$ and the ESR line shape depend on ionic motion. A change of the activation energy of $σ(T)$ at $125$ K coincides with the onset of the ionic DC conductivity. The ESR line shape is determined mainly by Li ionic motion within octahedral voids below $150$ K. At higher temperatures, fluctuations due to ionic diffusion change the environment of defects from axial to effectively isotropic on the ESR time scale. $σ(T)$ data up to $700$ K through the depolymerization transition confirm that the monomeric phase of Li$_4$C$_{60}$ is a metal.

cond-mat.str-el↗