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Paulina Plochocka

Publications and source records attributed to Paulina Plochocka.

At least 19 recordsLinked to original sources
arXiv2026

Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field

The coherent coupling of cavity-confined photons and excitonic matter resonances leads to the formation of cavity polaritons, hybrid light-matter quasi-particles. If multiple exciton resonances couple to the same photonic mode, the resulting polariton constitutes a coherent interaction between matter resonances that can be spatially separated without any direct electronic coupling. In this work, we demonstrate the formation of such a coherent coupling at room temperature using an open optical cavity containing two distinct van der Waals materials - monolayer WS2 and layered quasi-2D halide perovskites (HaPs) - separated by $1.5 μ\rm m$. The system forms three polariton branches, with the middle branch possessing nearly equal fractions of both excitons and the photonic mode. White-light reflectivity and luminescence measurements are in good agreement with simulations using a coupled harmonic oscillator and a microscopic Wannier-Hopfield framework. Our results lay the foundation to combine highly complementary degrees of freedom in 2D materials in an in-situ tunable fashion to enable new polaritonic functionalities.

cond-mat.mes-hall↗
arXiv2026

Geometry-Controlled Magnetic and Electronic Landscapes in Anisotropic van der Waals Materials

Electronic structure in van der Waals materials is commonly engineered through composition, strain, electrostatic gating and heterostructure assembly. Here we introduce geometronics, a concept in which substrate geometry locally reorients an anisotropic crystal, transforming homogeneous external perturbation into programmable magnetic and electronic landscapes. We demonstrate this concept using a bilayer of the antiferromagnetic semiconductor CrSBr transferred onto an inverted pyramidal nanoindentation, where the local crystal orientation with respect to the external magnetic field drives the coexistence of antiferromagnetic and ferromagnetic phases within a single continuous crystal. The resulting magnetic landscape creates a switchable excitonic potential well of up to 10--12 meV, directly visualised by spatially resolved spectroscopy. More generally, geometronics provides a universal route for deterministically programmed electronic and magnetic landscapes without modifying the material itself. It therefore establishes substrate topography as a new design principle that exploits the intrinsic anisotropy of layered van der Waals materials.

cond-mat.mtrl-sci↗
arXiv2026

Tunable Magneto-Excitonic Coupling in Alloyed van der Waals Antiferromagnet

The unique coupling between magnetic order and photo-generated excitons, electron-hole pairs bound by Coulomb interaction, in layered magnetic semiconductors offers a powerful mechanism for controlling light-matter interactions. In the van der Waals antiferromagnet CrSBr, this coupling is exceptionally strong and manifests distinctly between two coexisting excitonic states: the localised, Frenkel-like XA exciton and the more delocalised, Wannier-Mott-like XB exciton, providing a unique playground for the optical control of magnetism. Here, we reveal how chlorine incorporation reshapes the magneto-optical interplay in CrSBr1-xClx by simultaneously modifying its electronic structure, excitonic properties, and magnetic interactions. Combining magneto-optical spectroscopy up to 85 T with state-of-the-art quasiparticle self-consistent GW (QSGW) calculations on alloy supercells, we show that Cl insertion progressively localises the excitonic wavefunctions and drives both states toward a more Frenkel-like regime. This evolution is accompanied by a systematic reduction of the magnetic-field-induced energy renormalisation, most prominently for the XB exciton. Our work connects exciton character directly to magneto-excitonic coupling. Furthermore, it establishes compositional alloying as an effective strategy for engineering the coupling between magnetic and optical properties in van der Waals magnetic semiconductors.

cond-mat.mtrl-sci↗
arXiv2025

Spin injection and emission helicity switching in a 2D perovskite/WSe2 heterostructure

The initialization and control of a long-lived spin population in lead halide perovskites are prerequisites for their use in spintronic applications. Here, we demonstrate circular polarization of the interlayer exciton emission in a (BA)2PbI4/WSe2 monolayer heterostructure. The helicity of this emission is controlled by tuning the energy of the excitation laser through the manifold of exciton resonances of the WSe2 monolayer, together with an emerging interlayer absorption feature of the heterostructure. Theoretical calculations show that this resonance arises from hybridized (BA)2PbI4/WSe2 states in the valence band. This hybrid character enables its observation in both linear absorption and ultrafast pump-probe spectroscopies, and plays a key role in controlling the sign of the helicity of the interlayer exciton emission. The tunable spin polarization demonstrated here, with the WSe2 monolayer effectively acting as a tunable spin filter, represents an important step toward the use of 2D perovskites in opto-spintronic applications.

cond-mat.mtrl-sci↗
arXiv2025

Steric Engineering of Exciton Fine Structure in 2D Perovskites

A comprehensive study of excitonic properties of 2D layered perovskites is provided, with an emphasis on understanding and controlling the exciton fine structure. First, an overview of the optical properties is presented, discussing the challenges in determining the bandgap and exciton binding energies. Through magneto-optical spectroscopic measurements (up to B = 140 T), scaling laws are established for exciton binding energy as a function of the band gap and the diamagnetic coefficient. Using an in-plane magnetic field, the exciton fine structure for various 2D perovskites is examined to measure the energy splitting between the excitonic levels. The exciton fine structure and exchange interaction are correlated with structural parameters, employing an effective mass model, to highlight the role of steric effect on the exchange interaction. These findings reveal that lattice distortions, introduced by organic spacers, significantly influence the exchange interaction, driving a tunable energy spacing between dark and bright excitons. This unique feature of 2D perovskites, not present in other semiconductors, offers a novel tuning mechanism for exciton control, making these materials highly promising for efficient light emitters and advanced quantum technologies.

cond-mat.mtrl-sci↗
arXiv2025

Quadrupolar Excitons in MoSe$_2$ Bilayers

The quest for platforms to generate and control exotic excitonic states has greatly benefited from the advent of transition metal dichalcogenide (TMD) monolayers and their heterostructures. Among the unconventional excitonic states, quadrupolar excitons - a superposition of two dipolar excitons with anti-aligned dipole moments - are of great interest for applications in quantum simulations and for the investigation of many-body physics. Here, we unambiguously demonstrate the emergence of quadrupolar excitons in natural MoSe$_2$ homobilayers, whose energy shifts quadratically in electric field. In contrast to trilayer systems, MoSe$_2$ homobilayers have many advantages, which include a larger coupling between dipolar excitons. Our experimental observations are complemented by many-particle theory calculations offering microscopic insights in the formation of quadrupolar excitons. Our results suggest TMD homobilayers as ideal platform for the engineering of excitonic states and their interaction with light and thus candidate for carrying out on-chip quantum simulations.

cond-mat.mes-hall↗
arXiv2024

Approaching the Intrinsic Properties of Moiré Structures Using Atomic Force Microscopy Ironing

Stacking monolayers of transition metal dichalcogenides (TMDs) has led to the discovery of a plethora of new exotic phenomena, resulting from moiré pattern formation. Due to the atomic thickness and high surface-to-volume ratio of heterostructures, the interfaces play a crucial role. Fluctuations in the interlayer distance affect interlayer coupling and moiré effects. Therefore, to access the intrinsic properties of the TMD stack, it is essential to obtain a clean and uniform interface between the layers. Here, we show that this is achieved by ironing with the tip of an atomic force microscope. This post-stacking procedure dramatically improves the homogeneity of the interfaces, which is reflected in the optical response of the interlayer exciton. We demonstrate that ironing improves the layer coupling, enhancing moiré effects and reducing disorder. This is crucial for the investigation of TMD heterostructure physics, which currently suffers from low reproducibility.

cond-mat.mes-hall↗
arXiv2023

Phonon-bottleneck enhanced exciton emission in 2D perovskites

Layered halide perovskites exhibit remarkable optoelectronic properties and technological promise, driven by strongly bound excitons. The interplay of spin-orbit and exchange coupling creates a rich excitonic landscape, determining their optical signatures and exciton dynamics. Despite the dark excitonic ground state, surprisingly efficient emission from higher-energy bright states has puzzled the scientific community, sparking debates on relaxation mechanisms. Combining low-temperature magneto-optical measurements with sophisticated many-particle theory, we elucidate the origin of the bright exciton emission in perovskites by tracking the thermalization of dark and bright excitons under a magnetic field. We clearly attribute the unexpectedly high emission to a pronounced phonon-bottleneck effect, considerably slowing down the relaxation towards the energetically lowest dark states. We demonstrate that this bottleneck can be tuned by manipulating the bright-dark energy splitting and optical phonon energies, offering valuable insights and strategies for controlling exciton emission in layered perovskite materials that is crucial for optoelectronics applications.

cond-mat.mes-hall↗
arXiv2021

Photophysics of two-dimensional perovskites -- learning from metal halide substitution

Whereas their photophysics exhibits an intricate interplay of carriers with the lattice, most reports have so far relied on single compound studies. With the exception of variations of the organic spacer cations, the effect of constituent substitution on the photophysics and the nature of emitting species, in particular, has remained largely under-explored. Here PEA$_2$PbBr$_4$, PEA$_2$PbI$_4$, and PEA$_2$SnI$_4$ are studied through a variety of optical spectroscopy techniques to reveal a complex set of excitonic transitions at low temperature. We attribute the emergence of weak high energy features to a vibronic progression breaking Kasha's rule and highlight that the responsible phonons cannot be accessed through simple Raman spectroscopy. Bright peaks at lower energy are due to two distinct excitons, of which the upper is a convolution of a bright exciton and a localised state, whereas the lower is attributed to shallow defects. Our study offers deeper insights into the photophysics of two-dimensional perovskites through compositional substitution and highlights critical limits to the communities' current understanding of the photophysics of these compounds.

cond-mat.mtrl-sci↗
arXiv2020

Microscopic picture of electron-phonon interaction in two-dimensional halide perovskites

Perovskites have attracted much attention due to their remarkable optical properties. While it is well established that excitons dominate their optical response, the impact of higher excitonic states and formation of phonon sidebands in optical spectra still need to be better understood. Here, we perform a theoretical study on excitonic properties of monolayered hybrid organic perovskites -- supported by temperature-dependent photoluminescence measurements. Solving the Wannier equation, we obtain microscopic access to the Rydberg-like series of excitonic states including their wavefunctions and binding energies. Exploiting the generalized Elliot formula, we calculate the photoluminescence spectra demonstrating a pronounced contribution of a phonon sideband for temperatures up to 50 K -- in agreement with experimental measurements. Finally, we predict temperature-dependent linewidths of the three energetically lowest excitonic transitions and identify the underlying phonon-driven scattering processes.

cond-mat.mes-hall↗
arXiv2020

Symmetry breakdown in franckeite: spontaneous strain, rippling and interlayer moiré

Franckeite is a naturally occurring layered mineral with a structure composed of alternating stacks of SnS2-like and PbS-like layers. Although this superlattice is composed of a sequence of isotropic two-dimensional layers, it exhibits a spontaneous rippling that makes the material structurally anisotropic. We demonstrate that this rippling comes hand in hand with an inhomogeneous in-plane strain profile and anisotropic electrical, vibrational and optical properties. We argue that this symmetry breakdown results from a spatial modulation of the van der Waals interaction between layers due to the SnS2-like and PbS-like lattices incommensurability.

cond-mat.mes-hall↗
arXiv2020

The impact of hexagonal boron nitride encapsulation on the structural and vibrational properties of few layer black phosphorus

The encapsulation of two-dimensional layered materials such as black phosphorus is of paramount importance for their stability in air. However, the encapsulation poses several questions, namely, how it affects, via the weak van der Waals forces, the properties of the black phosphorus and whether these properties can be tuned on demand. Prompted by these questions, we have investigated the impact of hexagonal boron nitride encapsulation on the structural and vibrational properties of few layer black phosphorus, using a first-principles method in the framework of density functional theory. We demonstrate that the encapsulation with hexagonal boron nitride imposes biaxial strain on the black phosphorus material, flattening its puckered structure, by decreasing the thickness of the layers via the increase of the puckered angle and the intra-layer P-P bonds. This work exemplifies the evolution of structural parameters in layered materials after the encapsulation process. We find that after encapsulation, phosphorene (single layer black phosphorous) contracts by 1.1% in the armchair direction and stretches by 1.3% in the zigzag direction, whereas few layer black phosphorus mainly expands by up to 3% in the armchair direction. However, these relatively small strains induced by the hexagonal BN, lead to significant changes in the vibrational properties of black phosphorus, with the redshifts of up to 10 cm$^{-1}$ of the high frequency optical mode $A_g^1$. In general, structural changes induced by the encapsulation process open the door to substrate controlled strain engineering in two-dimensional crystals.

cond-mat.mtrl-sci↗
arXiv2019

Giant Fine Structure Splitting of the Bright Exciton in a Bulk MAPbBr$_3$ Single Crystal

Exciton fine structure splitting in semiconductors reflects the underlying symmetry of the crystal and quantum confinement. Since the latter factor strongly enhances the exchange interaction, most work has focused on nanostructures. Here, we report on the first observation of the bright exciton fine structure splitting in a bulk semiconductor crystal, where the impact of quantum confinement can be specifically excluded, giving access to the intrinsic properties of the material. Detailed investigation of the exciton photoluminescence and reflection spectra of a bulk methylammonium lead tribromide single crystal reveals a zero magnetic field splitting as large as $\sim 200μ$eV. This result provides an important starting point for the discussion of the origin of the large bright exciton fine structure observed in perovskite nanocrystals.

cond-mat.mes-hall↗
arXiv2019

Phase Transition Induced Carrier Mass Enhancement in 2D Ruddlesden-Popper Perovskites

There is a variety of possible ways to tune the optical properties of 2D perovskites, though the mutual dependence between different tuning parameters hinders our fundamental understanding of their properties. In this work we attempt to address this issue for (C$_n$H$_{2n+1}$NH$_3$)$_2$PbI$_4$ (with n=4,6,8,10,12) using optical spectroscopy in high magnetic fields up to 67T. Our experimental results, supported by DFT calculations, clearly demonstrate that the exciton reduced mass increases by around 30% in the low temperature phase. This is reflected by a 2-3 fold decrease of the diamagnetic coefficient. Our studies show that the effective mass, which is an essential parameter for optoelectronic device operation, can be tuned by the variation of organic spacers and/or moderate cooling achievable using Peltier coolers. Moreover, we show that the complex absorption features visible in absorption/transmission spectra track each other in magnetic field providing strong evidence for the phonon related nature of the observed side bands.

cond-mat.mes-hall↗
arXiv2018

Moiré Intralayer Excitons in a MoSe$_2$/MoS$_2$ Heterostructure

Spatially periodic structures with a long range period, referred to as moiré pattern, can be obtained in van der Waals bilayers in the presence of a small stacking angle or of lattice mismatch between the monolayers. Theoretical predictions suggest that the resulting spatially periodic variation of the band structure modifies the optical properties of both intra and interlayer excitons of transition metal dichalcogenides heterostructures. Here, we report on the impact of the moiré pattern formed in a MoSe$_2$/MoS$_2$ heterobilayer encapsulated in hexagonal boron nitride. The periodic in-plane potential results in a splitting of the MoSe$_2$ exciton and trion in both emission and absorption spectra. The observed energy difference between the split peaks is fully consistent with theoretical predictions.

cond-mat.mes-hall↗
arXiv2018

Intervalley Scattering of Interlayer Excitons in a MoS$_2$/MoSe$_2$/MoS$_2$ Heterostructure in High Magnetic Field

Degenerate extrema in the energy dispersion of charge carriers in solids, also referred to as valleys, can be regarded as a binary quantum degree of freedom, which can potentially be used to implement valleytronic concepts in van der Waals heterostructures based on transition metal dichalcogenides. Using magneto-photoluminescence spectroscopy, we achieve a deeper insight into the valley polarization and depolarization mechanisms of interlayer excitons formed across a MoS$_2$/MoSe$_2$/MoS$_2$ heterostructure. We account for the non-trivial behavior of the valley polarization as a function of the magnetic field by considering the interplay between exchange interaction and phonon mediated intervalley scattering in a system consisting of Zeeman-split energy levels. Our results represent a crucial step towards the understanding of the properties of interlayer excitons, with strong implications for the implementation of atomically thin valleytronic devices.

cond-mat.mes-hall↗
arXiv2018

Probing Landau levels of strongly interacting massive Dirac electrons in layer-polarized MoS$_2$

Monolayer transition metal dichalcogenides are recently emerged 2D electronic systems with various novel properties, such as spin-valley locking, circular dichroism, valley Hall effects, Ising superconductivity. The reduced dimensionality and large effective masses further produce unconventional many-body interaction effects. Although recent hole transport measurements in WSe$_2$ indicate strong interactions in the valence bands, many-body interaction effects, particularly in the conduction bands, remain elusive to date. Here, for the first time, we perform transport measurements up to a magnetic field of $29$T to study the massive Dirac electron Landau levels (LL) in layer-polarized MoS$_2$ samples with mobilities of $22000$cm$^2$/(V$\cdot$s) at $1.5$K and densities of $\sim10^{12}$cm$^{-2}$. With decreasing the density, we observe LL crossing induced valley ferrimagnet-to-ferromagnet transitions, as a result of the interaction enhancement of the g-factor from $5.64$ to $21.82$. Near integer ratios of Zeeman-to-cyclotron energies, we discover LL anticrossings due to the formation of quantum Hall Ising ferromagnets, the valley polarizations of which appear to be reversible by tuning the density or an in-plane magnetic field. Our results provide compelling evidence for many-body interaction effects in the conduction bands of monolayer MoS$_2$ and establish a fertile ground for exploring strongly correlated phenomena of massive Dirac electrons.

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