arXiv subjects

Paulina Plochocka

Publications and source records attributed to Paulina Plochocka.

26 records · Page 2Linked to original sources

arXiv2018

Site-selective measurement of coupled spin pairs in an organic semiconductor

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site-sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet (S=0) and dark triplet, quintet (S=1,2) configurations: this induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3-5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site-selectivity can be achieved for organic spin pairs in a broad range of systems.

physics.chem-ph↗

arXiv2017

Defect healing and charge transfer mediated valley polarization in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures

Monolayer transition metal dichalcogenides (TMDC) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDC. In this work we show that the optical quality of CVD-grown MoSe$_2$ is completely recovered if the material is sandwiched in MoS$_2$/MoSe$_2$/MoS$_2$ trilayer van der Waals heterostructures. We show by means of density-functional theory that this remarkable and unexpected result is due to defect healing: S atoms of the more reactive MoS$_2$ layers are donated to heal Se vacancy defects in the middle MoSe$_2$ layer. In addition, the trilayer structure exhibits a considerable charge-transfer mediated valley polarization of MoSe$_2$ without the need for resonant excitation. Our fabrication approach, relying solely on simple flake transfer technique, paves the way for the scalable production of large-area TMDC materials with excellent optical quality.

cond-mat.mes-hall↗

arXiv2017

Highly-Oriented Atomically Thin Ambipolar MoSe$_2$ Grown by Molecular Beam Epitaxy

Transition metal dichalcogenides (TMDCs), together with other two-dimensional (2D) materials have attracted great interest due to the unique optical and electrical properties of atomically thin layers. In order to fulfill their potential, developing large-area growth and understanding the properties of TMDCs have become crucial. Here, we used molecular beam epitaxy (MBE) to grow atomically thin MoSe$_2$ on GaAs(111)B. No intermediate compounds were detected at the interface of as-grown films. Careful optimization of the growth temperature can result in the growth of highly aligned films with only two possible crystalline orientations due to broken inversion symmetry. As-grown films can be transferred onto insulating substrates allowing their optical and electrical properties to be probed. By using polymer electrolyte gating, we have achieved ambipolar transport in MBE-grown MoSe$_2$. The temperature-dependent transport characteristics can be explained by the 2D variable-range hopping (2D-VRH) model, indicating that the transport is strongly limited by the disorder in the film.

cond-mat.mtrl-sci↗

arXiv2017

Unraveling the exciton binding energy and the dielectric constant in single crystal methylammonium lead tri-iodide perovskite

We have accurately determined the exciton binding energy and reduced mass of single crystals of methylammonium lead tri-iodide using magneto-reflectivity at very high magnetic fields. The single crystal has excellent optical properties with a narrow line width of $\sim 3$meV for the excitonic transitions and a 2s transition which is clearly visible even at zero magnetic field. The exciton binding energy of $16 \pm 2$meV in the low temperature orthorhombic phase is almost identical to the value found in polycrystalline samples, crucially ruling out any possibility that the exciton binding energy depends on the grain size. In the room temperature tetragonal phase, an upper limit for the exciton binding energy of $12 \pm 4$ meV is estimated from the evolution of 1s-2s splitting at high magnetic field.

cond-mat.mtrl-sci↗

arXiv2015

Determination of the exciton binding energy and effective masses for the methylammonium and formamidinium lead tri-halide perovskite family

The family of organic-inorganic halide perovskite materials has generated tremendous interest in the field of photovoltaics due to their high power conversion efficiencies. There has been intensive development of cells based on the archetypal methylammonium (MA)and recently introduced formamidinium (FA) materials, however, there is still considerable controversy over their fundamental electronic properties. Two of the most important parameters are the binding energy of the exciton (R$^{*}$) and its reduced effective mass $μ$. Here we present extensive magneto optical studies of Cl assisted grown MAPbI$_{3}$ as well as MAPbBr$_{3}$ and the FA based materials FAPbI$_{3}$ and FAPbBr$_{3}$. We fit the excitonic states as a hydrogenic atom in magnetic field and the Landau levels for free carriers to give R$^{*}$ and $μ$. The values of the exciton binding energy are in the range 14 - 25 meV in the low temperature phase and fall considerably at higher temperatures for the tri-iodides, consistent with free carrier behaviour in all devices made from these materials. Both R$^{*}$ and $μ$ increase approximately proportionally to the band gap, and the mass values, 0.09-0.117 m$_{0}$, are consistent with a simple \textbf{k.p} perturbation approach to the band structure which can be generalized to predict values for the effective mass and binding energy for other members of this perovskite family of materials.

cond-mat.mes-hall↗

arXiv2015

Direct Measurement of the Exciton Binding Energy and Effective Masses for Charge carriers in an Organic-Inorganic Tri-halide Perovskite

Solar cells based on the organic-inorganic tri-halide perovskite family of materials have shown remarkable progress recently, offering the prospect of low-cost solar energy from devices that are very simple to process. Fundamental to understanding the operation of these devices is the exciton binding energy, which has proved both difficult to measure directly and controversial. We demonstrate that by using very high magnetic fields it is possible to make an accurate and direct spectroscopic measurement of the exciton binding energy, which we find to be only 16 meV at low temperatures, over three times smaller than has been previously assumed. In the room temperature phase we show that the binding energy falls to even smaller values of only a few millielectronvolts, which explains their excellent device performance due to spontaneous free carrier generation following light absorption. Additionally, we determine the excitonic reduced effective mass to be 0.104me (where me is the electron mass), significantly smaller than previously estimated experimentally but in good agreement with recent calculations. Our work provides crucial information about the photophysics of these materials, which will in turn allow improved optoelectronic device operation and better understanding of their electronic properties.

cond-mat.mes-hall↗

arXiv2012

Carrier dynamics in epitaxial graphene close to the Dirac point

We study the carrier dynamics in epitaxially grown graphene in the range of photon energies from 10 - 250 meV. The experiments complemented by microscopic modeling reveal that the carrier relaxation is significantly slowed down as the photon energy is tuned to values below the optical phonon frequency, however, owing to the presence of hot carriers, optical phonon emission is still the predominant relaxation process. For photon energies about twice the value of the Fermi energy, a transition from pump-induced transmission to pump-induced absorption occurs due to the interplay of interband and intraband processes.

cond-mat.mtrl-sci↗

arXiv2008

Approaching the Dirac point in high mobility multi-layer epitaxial graphene

Multi-layer epitaxial graphene (MEG) is investigated using far infrared (FIR) transmission experiments in the different limits of low magnetic fields and high temperatures. The cyclotron-resonance like absorption is observed at low temperature in magnetic fields below 50 mT, allowing thus to probe the nearest vicinity of the Dirac point and to estimate the conductivity in nearly undoped graphene. The carrier mobility is found to exceed 250,000 cm$^2$/(V.s). In the limit of high temperatures, the well-defined Landau level (LL) quantization is observed up to room temperature at magnetic fields below 1 T, a phenomenon unique in solid state systems. A negligible increase in the width of the cyclotron resonance lines with increasing temperature indicates that no important scattering mechanism is thermally activated, supporting recent expectations of high room-temperature mobilities in graphene.

cond-mat.other↗