arXiv subjects

V. Dyakonov

Publications and source records attributed to V. Dyakonov.

At least 37 records · Page 2Linked to original sources

arXiv2014

Engineering near infrared single photon emitters in ultrapure silicon carbide

Quantum emitters hosted in crystalline lattices are highly attractive candidates for quantum information processing, secure networks and nanosensing. For many of these applications it is necessary to have control over single emitters with long spin coherence times. Such single quantum systems have been realized using quantum dots, colour centres in diamond, dopants in nanostructures and molecules . More recently, ensemble emitters with spin dephasing times on the order of microseconds and room-temperature optically detectable magnetic resonance have been identified in silicon carbide (SiC), a compound being highly compatible to up-to-date semiconductor device technology. So far however, the engineering of such spin centres in SiC on single-emitter level has remained elusive. Here, we demonstrate the control of spin centre density in ultrapure SiC over 8 orders of magnitude, from below $10^{9}$ to above $10^{16} \,$cm$^{-3}$ using neutron irradiation. For a low irradiation dose, a fully photostable, room-temperature, near infrared (NIR) single photon emitter can clearly be isolated, demonstrating no bleaching even after $10^{14}$ excitation cycles. Based on their spectroscopic fingerprints, these centres are identified as silicon vacancies, which can potentially be used as qubits, spin sensors and maser amplifiers.

cond-mat.mtrl-sci↗

arXiv2014

Persistent photovoltage in methylammonium lead iodide perovskite solar cells

Open circuit voltage decay measurements are performed on methylammonium lead iodide (CH3NH3PbI3) perovskite solar cells to investigate the charge carrier recombination dynamics. The measurements are compared to the two reference polymer-fullerene bulk heterojunction solar cells based on P3HT:PC60BM and PTB7:PC70BM blends. In the perovskite devices, two very different time domains of the voltage decay are found, with a first drop on a short time scale that is similar to the organic solar cells. However, two major differences are also observed. 65-70% of the maximum photovoltage persists on much longer timescales, and the recombination dynamics are dependent on the illumination intensity.

cond-mat.mtrl-sci↗

arXiv2014

Excitation and recombination dynamics of vacancy-related spin centers in silicon carbide

We generate silicon vacancy related defects in high-quality epitaxial silicon carbide layers by means of electron irradiation. By controlling the irradiation fluence, the defect concentration is varied over several orders of magnitude. We establish the excitation profile for optical pumping of these defects and evaluate the optimum excitation wavelength of 770 nm. We also measure the photoluminescence dynamics at room temperature and find a monoexponential decay with a characteristic lifetime of 6.1 ns. The integrated photoluminescence intensity depends linear on the excitation power density up to 20 kW/cm$^2$, indicating a relatively small absorption cross section of these defects.

cond-mat.mtrl-sci↗

arXiv2014

Magnetic field and temperature sensing with atomic-scale spin defects in silicon carbide

Quantum systems can provide outstanding performance in various sensing applications, ranging from bioscience to nanotechnology. Atomic-scale defects in silicon carbide are very attractive in this respect because of the technological advantages of this material and favorable optical and radio frequency spectral ranges to control these defects. We identified several, separately addressable spin-3/2 centers in the same silicon carbide crystal, which are immune to nonaxial strain fluctuations. Some of them are characterized by nearly temperature independent axial crystal fields, making these centers very attractive for vector magnetometry. Contrarily, the zero-field splitting of another center exhibits a giant thermal shift of -1.1 MHz/K at room temperature, which can be used for thermometry applications. We also discuss a synchronized composite clock exploiting spin centers with different thermal response.

cond-mat.mtrl-sci↗

arXiv2012

Intrinsic defects in silicon carbide LED as a perspective room temperature single photon source in near infrared

Generation of single photons has been demonstrated in several systems. However, none of them satisfies all the conditions, e.g. room temperature functionality, telecom wavelength operation, high efficiency, as required for practical applications. Here, we report the fabrication of light emitting diodes (LEDs) based on intrinsic defects in silicon carbide (SiC). To fabricate our devices we used a standard semiconductor manufacturing technology in combination with high-energy electron irradiation. The room temperature electroluminescence (EL) of our LEDs reveals two strong emission bands in visible and near infrared (NIR), associated with two different intrinsic defects. As these defects can potentially be generated at a low or even single defect level, our approach can be used to realize electrically driven single photon source for quantum telecommunication and information processing.

cond-mat.mtrl-sci↗

arXiv2012

Magnetic anisotropy of La0.7Sr0.3MnO3 nanopowders

The magnetic anisotropy of La0.7Sr0.3MnO3 nanopowders was measured as a function of temperature by the modified singular point detection technique. In this method singularities indicating the anisotropy field were determined analyzing ac susceptibility data. The observed relationship between temperature dependence of anisotropy constant and temperature dependence of magnetization was used to deduce the origin of magnetic anisotropy in the nanopowders. It was shown that magnetic anisotropy of La0.7Sr0.3MnO3 nanopowder is determined by two-ion (dipolar or pseudodipolar) and single-ion mechanisms.

cond-mat.mtrl-sci↗

arXiv2012

Resonant addressing and manipulation of silicon vacancy qubits in silicon carbide

Several systems in the solid state have been suggested as promising candidates for spin-based quantum information processing. In spite of significant progress during the last decade, there is a search for new systems with higher potential [D. DiVincenzo, Nature Mat. 9, 468 (2010)]. We report that silicon vacancy defects in silicon carbide comprise the technological advantages of semiconductor quantum dots and the unique spin properties of the nitrogen-vacancy defects in diamond. Similar to atoms, the silicon vacancy qubits can be controlled under the double radio-optical resonance conditions, allowing for their selective addressing and manipulation. Furthermore, we reveal their long spin memory using pulsed magnetic resonance technique. All these results make silicon vacancy defects in silicon carbide very attractive for quantum applications.

cond-mat.mtrl-sci↗

arXiv2012

Shockley Equation Parameters of Organic Solar Cells derived by Transient Techniques

The Shockley equation (SE), originally derived to describe a p--n junction, was frequently used in the past to simulate current--voltage (j/V) characteristics of organic solar cells (OSC). In order to gain a more detailed understanding of recombination losses, we determined the SE parameters, i.e. the ideality factor and the dark saturation current, from temperature dependent static j/V-measurements on poly(3-hexylthiophene-2,5-diyl)(P3HT):[6,6]-phenyl-C$_{61}$ butyric acid methyl ester (PCBM) bulk heterojunction solar cells. As we show here, these parameters are directly related to charge carrier recombination and become also accessible by transient photovoltage and photocurrent methods in the case of field-independent charge carrier generation. Although determined in very different ways, both SE parameters were found to be identical. The good agreement of static and transient approaches over a wide temperature range demonstrates the validity of the Shockley model for OSC based on material systems satisfying the requirement of field-independent polaron-pair dissociation. In particular, we were able to reproduce the photocurrent at various light intensities and temperatures from the respective nongeminate recombination rates. Furthermore, the temperature dependence of the dark saturation current $j_0$ allowed determining the effective band gap of the photoactive blend perfectly agreeing with the literature values of the energy onset of the photocurrent due to charge transfer absorption. We also present a consistent model directly relating the ideality factor to recombination of free with trapped charge carriers in an exponential density of tail states. We verify this finding by data from thermally stimulated current measurements.

cond-mat.mtrl-sci↗

arXiv2012

Charge density dependent nongeminate recombination in organic bulk heterojunction solar cells

Apparent recombination orders exceeding the value of two expected for bimolecular recombination have been reported for organic solar cells in various publications. Two prominent explanations are bimolecular losses with a carrier concentration dependent prefactor due to a trapping limited mobility, and protection of trapped charge carriers from recombination by a donor--acceptor phase separation until reemission from these deep states. In order to clarify which mechanism is dominant we performed temperature and illumination dependent charge extraction measurements under open circuit as well as short circuit conditions at poly(3-hexylthiophene-2,5-diyl):[6,6]-phenyl-C$_{61}$butyric acid methyl ester (P3HT:PC$_{61}$BM) and PTB7:PC$_{71}$BM (Poly[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b]thiophenediyl]]) solar cells in combination with current--voltage characteristics. We show that the charge carrier density $n$ dependence of the mobility $μ$ and the recombination prefactor are different for PC$_{61}$BM at temperatures below 300K and PTB7:PC$_{71}$BM at room temperature. Therefore, in addition to $μ(n)$ a detrapping limited recombination in systems with at least partial donor--acceptor phase separation is required to explain the high recombination orders.

cond-mat.soft↗

arXiv2010

Role of Polaron Pair Diffusion and Surface Losses in Organic Semiconductor Devices

By applying Monte Carlo simulations we found that the extraction of bound polaron pairs (PP) at the electrodes is an important loss factor limiting the efficiency of organic optoelectronic and photovoltaic devices. Based upon this finding, we developed a unified analytic model consisting of exact Onsager theory, describing the dissociation of PP in organic donor-acceptor heterojunctions, the Sokel-Hughes model for the extraction of free polarons at the electrodes, as well as of PP diffusion leading to the aforementioned loss mechanism, which was not considered previously. Our approach allows to describe the simulation details on a macroscopic scale and to gain fundamental insights, which is important in view of developing an optimized photovoltaic device configuration.

cond-mat.mtrl-sci↗

arXiv2010

S-shaped current-voltage characteristics of organic solar devices

Measuring the current-voltage characteristic of organic bulk heterojunction solar devices sometimes reveals an s-shaped deformation. We qualitatively produce this behaviour by a numerical device simulation assuming a reduced surface recombination. Furthermore we show how to experimentally create these double diodes by applying an oxygen plasma etch on the indium tin oxide (ITO) anode. Restricted charge transport over material interfaces accumulates space charges and therefore creates s-shaped deformations. Finally we discuss the consequences of our findings for the open circuit voltage $V_{oc}$

cond-mat.mtrl-sci↗

arXiv2010

Spectroscopic Signatures of Photogenerated Radical Anions in Polymer-[C70]Fullerene Bulk Heterojunctions

Light induced polarons in solid films of polymer-fullerene blends were studied by applying photoluminescence (PL), photo induced absorption (PIA) techniques as well as electron spin resonance (ESR). The materials used were poly(3-hexylthiophene) (P3HT) and poly-[2-methoxy, 5-(2'-ethyl-hexyloxy) phenylene vinylene] (MEH-PPV) as donors. As acceptors we used [6,6]-phenyl-C61-butyric acid methyl ester ([C60]PCBM) and various soluble C70-derivates: [C70]PCBM, diphenylmethano[70]fullerene oligoether (C70-DPM-OE), C70-DPM-OE2, and two fullerene dimers, C70-C70 and C60-C70 (all shown in figure 1). In all blends containing C70 we found typical signatures which were absent if [C60]PCBM was used as acceptor. Light-induced ESR revealed signals at g>=2.005, which we previously assigned to an electron localized on the C70 cage, the PIA measurements showed a new sub-bandgap absorption band at 0.92 eV, which we correspondingly ascribe to C70 radical anions formed in the course of photoinduced electron transfer from donor to acceptor.

cond-mat.mtrl-sci↗

arXiv2010

Organic solar cell efficiencies under the aspect of reduced surface recombination velocities

The charge carrier mobility is a key parameter for the organic bulk heterojunction solar cell efficiency. It was recently shown that the interplay charge carrier transport and recombination, both depending on electron and hole mobilities, leads to a point of maximum power conversion efficiency at a finite mobility. Changes of bulk and surface recombination rate, however, can strongly influence this behavior. These processes were previously not considered adequately, as surface recombination velocities of infinity were implicitly assumed or bulk recombination parameters not discussed in detail. In this manuscript, using a macroscopic effective medium simulation, we consider how a reduced bulk recombination process in combination with finite surface recombination velocities affect the power conversion efficiency. Instead of a maximum efficiency at a specific charge carrier mobility, we show that with realistic assumptions and passivated surfaces the efficiency is increased further, saturating only at higher mobilities. Thus, a mobility optimisation is more important for the solar cell performance then previously shown.

cond-mat.mtrl-sci↗

arXiv2010

Investigation of the Photocurrent in Bulk Heterojunction Solar Cells

We investigated the photocurrent in poly(3-hexylthiophene-2,5-diyl) (P3HT):[6,6]-phenyl-C$_{61}$ butyric acid methyl ester (PCBM) solar cells by applying a pulsed measurement technique. For annealed samples, a point of optimal symmetry (POS) with a corresponding voltage $V_\text{POS}$ of 0.52--0.64 V could be determined. Based on macroscopic simulations and results from capacitance--voltage measurements, we identify this voltage with flat band conditions in the bulk of the cell, but not the built-in voltage as proposed by [Ooi et al., J. Mater. Chem. 18 (2008) 1644]. We calculated the field dependent polaron pair dissociation after Onsager--Braun and the voltage dependent extraction of charge carriers after Sokel and Hughes with respect to this point of symmetry. Our analysis allows to explain the experimental photocurrent in both forward and reverse directions. Also, we observed a voltage--independent offset of the photocurrent. As this offset is crucial for the device performance, we investigated its dependence on cathode material and thermal treatment. From our considerations we gain new insight into the photocurrent`s voltage dependence and the limitations of device efficiency.

cond-mat.mtrl-sci↗

arXiv2009

Origin of the Efficient Polaron Pair Dissociation in Polymer--Fullerene Blends

The separation of photogenerated polaron pairs in organic bulk heterojunction solar cells is the intermediate but crucial step between exciton dissociation and charge transport to the electrodes. In state-of-the-art devices, above 80% of all polaron pairs are separated at fields of below $10^7$V/m. In contrast, considering just the Coulomb binding of the polaron pair, electric fields above $10^8$V/m would be needed to reach similar yields. In order to resolve this discrepancy, we performed kinetic Monte Carlo simulations of polaron pair dissociation in donor--acceptor blends, considering delocalised charge carriers along conjugated polymer chain segments. We show that the resulting fast local charge carrier transport can indeed explain the high experimental quantum yields in polymer solar cells.

cond-mat.mtrl-sci↗

arXiv2009

Polaron Recombination in Pristine and Annealed Bulk Heterojunction Solar Cells

The major loss mechanism of photogenerated polarons was investigated in P3HT:PCBM solar cells by the photo-CELIV technique. For pristine and annealed devices, we find that the experimental data can be explained by a bimolecular recombination rate reduced by a factor of about ten (pristine) and 25 (annealed) as compared to Langevin theory. Aided by a macroscopic device model, we discuss the implications of the lowered loss rate on the characteristics of polymer:fullerene solar cells.

cond-mat.mtrl-sci↗

arXiv2009

Origin of Reduced Polaron Recombination in Organic Semiconductor Devices

We propose a model to explain the reduced bimolecular recombination rate found in state-of-the-art bulk heterojunction solar cells. When compared to the Langevin recombination, the experimentally observed rate is one to four orders of magnitude lower, but gets closer to the Langevin case for low temperatures. Our model considers the organic solar cell as device with carrier concentration gradients, which form due to the electrode/blend/electrode device configuration. The resulting electron concentration under working conditions of a solar cell is higher at the cathode than at the anode, and vice versa for holes. Therefore, the spatially dependent bimolecular recombination rate, proportional to the local product of electron and hole concentration, is much lower as compared to the calculation of the recombination rate based on the extracted and thus averaged charge carrier concentrations. We consider also the temperature dependence of the recombination rate, which can for the first time be described with our model.

cond-mat.mtrl-sci↗

arXiv2009

Charge Carrier Concentration and Temperature Dependent Recombination in Polymer Fullerene Solar Cells

We performed temperature dependent transient photovoltage and photocurrent measurements on poly(3-hexylthiophene):[6,6]-phenyl-C61 butyric acid methylester bulk heterojuction solar cells. We found a strongly charge carrier concentration and temperature dependent Langevin recombination prefactor. The observed recombination mechanism is discussed in terms of bimolecular recombination. The experimental results were compared with charge carrier extraction by linearly increasing voltage (photo-CELIV) measurements done on the same blend system. We explain the charge carrier dynamics, following an apparent order larger than two, by dynamic trapping of charges in the tail states of the gaussian density of states.

cond-mat.mtrl-sci↗