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S. Kollarics

Publications and source records attributed to S. Kollarics.

14 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

A Versatile System for Photoconductance Decay Measurement Across a Wide Range of Semiconductor Materials

Time-resolved photoconductivity is widely used to characterize non-equilibrium charge-carrier lifetime, impurity content, and solar cell efficiency in a broad range of semiconductors. Most measurements are limited to the detection of reflection of electromagnetic radiation at a single frequency and a single photoexciting light wavelength. We present a time-resolved photoconductivity instrument that enables broadband frequency detection (essentially from DC to 100 GHz), temperature-dependent measurements, and multiple excitation photon energy. The measurement is realized with the help of a coplanar waveguide, which acts as an efficient antenna and whose performance was tested over 10 MHz-10 GHz. The instrument enables the study of surface and bulk charge-recombination specific processes.

cond-mat.mtrl-sci

Dynamics of Photoinduced Charge Carriers in Metal-Halide Perovskites

The measurement and description of the charge-carrier lifetime (tauc) is crucial for the wide-ranging applications of lead-halide perovskites. We present time-resolved microwave-detected photoconductivity decay (TRMCD) measurements and a detailed analysis of the possible recombination mechanisms including trap-assisted, radiative, and Auger recombination. We prove that performing injection-dependent measurement is crucial in identifying the recombination mechanism. We present temperature and injection level dependent measurements in CsPbBr_3, which is an inorganic lead-halide perovskite. In this material, we observe the dominance of charge-carrier trapping, which results in ultra-long charge-carrier lifetimes. Although charge trapping can limit the effectiveness of materials in photovoltaic applications, it also offers significant advantages for various alternative uses, including delayed and persistent photodetection, charge-trap memory, afterglow light-emitting diodes, quantum information storage, and photocatalytic activity.

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

Ultra-long charge carrier recombination time in methylammonium lead halide perovskites

Due to their exceptional photovoltaic properties, metal halide perovskites (MHPs) are extensively studied for their potential applications in solar cells. In recent years, the power conversion efficiencies of MHPs-based solar cells rapidly increased from the initial few \% towards more than 25\,\% for single-junction devices. Therefore, also taking into account their low costs and ease of manufacturing, MHPs-based solar cells have become the fastest-advancing photovoltaic technology. In this regard, much of the recent work has been dominated by absorber materials based on methylammonium MHPs, such as MAPbX$_3$, where MA=CH$_3$NH$_3$ and X=Cl, Br and I. Here, we present the results of contactless time-resolved photoconductivity measurements in an exceptionally wide range of temperatures of $4$ to $290\ \text{K}$ that were performed for the various crystalline forms of the three parent MAPbX$_3$, i.e., MAPbCl$_3$, MAPbBr$_3$ and MAPbI$_3$. This approach was made possible by the use of a high quality-factor (Q) microwave resonator, which cooperated with a commercially available microwave bridge equipped with an automatic frequency control (AFC) and a helium gas-flow cryostat.

cond-mat.mtrl-sci

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

Incidence of Quantum Confinement on Dark Triplet Excitons in Carbon Nanotubes

Photophysics of single-wall carbon nanotubes (SWCNTs) is intensively studied due to their potential application in light harvesting and optoelectronics. Excited states of SWCNTs form strongly bound electron-hole pairs, excitons, of which only singlet excitons participate in application relevant optical transitions. Long-living spin-triplet states hinder applications but they emerge as candidates for quantum information storage. Therefore knowledge of the triplet exciton energy structure, in particular in a SWCNT chirality dependent manner, is greatly desired. We report the observation of light emission from triplet state recombination, i.e. phosphorescence, for several SWCNT chiralities using a purpose-built spectrometer. This yields the singlet-triplet gap as a function of SWCNT diameter and it follows predictions based on quantum confinement effects. Saturation under high microwave power (up to 10 W) irradiation allows to determine the spin-relaxation time for triplet states. Our study sensitively discriminates whether the lowest optically active state is populated from an excited state on the same nanotube or through Förster exciton energy transfer from a neighboring nanotube.

cond-mat.mes-hall

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

Non-exponential magnetic relaxation in magnetic nanoparticles for hyperthermia

Magnetic nanoparticle based hyperthermia emerged as a potential tool for treating malignant tumours. The efficiency of the method relies on the knowledge of magnetic properties of the samples; in particular, knowledge of the frequency dependent complex magnetic susceptibility is vital to optimize the irradiation conditions and to provide feedback for material science developments. We study the frequency-dependent magnetic susceptibility of an aqueous ferrite suspension for the first time using non-resonant and resonant radiofrequency reflectometry. We identify the optimal measurement conditions using a standard solenoid coil, which is capable of providing the complex magnetic susceptibility up to 150 MHz. The result matches those obtained from a radiofrequency resonator for a few discrete frequencies. The agreement between the two different methods validates our approach. Surprisingly, the dynamic magnetic susceptibility cannot be explained by an exponential magnetic relaxation behavior even when we consider a particle size-dependent distribution of the relaxation parameter.

physics.app-ph

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

An optically detected magnetic resonance spectrometer with tunable laser excitation and wavelength resolved infrared detection

We present the development and performance of an optically detected magnetic resonance (ODMR) spectrometer. The spectrometer represents advances over similar instruments in three areas: i) the exciting light is a tunable laser source which covers much of the visible light range, ii) the optical signal is analyzed with a spectrograph, iii) the emitted light is detected in the near-infrared domain. The need to perform ODMR experiments on single-walled carbon nanotubes motivated the present development and we demonstrate the utility of the spectrometer on this material. The performance of the spectrometer is critically compared to similar instruments. The present development opens the way to perform ODMR studies on various new materials such as molecules and luminescent quantum dots where the emission is in the near-infrared range and requires a well-defined excitation wavelength and analysis of the scattered light.

physics.ins-det