arXiv subjects

Maciej Koperski

Publications and source records attributed to Maciej Koperski.

At least 19 recordsLinked to original sources

arXiv2026

Manipulation of localized excitons in CrPS$_4$ by temperature and magnetic field

Layered van der Waals magnetic semiconductors provide a versatile platform for exploring excitonic phenomena intertwined with spin and lattice degrees of freedom, enabling excitons to act as sensitive probes of magnetic order. CrPS$_4$ is a layered antiferromagnetic semiconductor that hosts rich excitonic features whose microscopic origin and connection to magnetic ordering remain incompletely understood. Here, we investigate the electronic and excitonic properties of bulk CrPS$_4$ using a combination of many-body perturbation theory, dynamical mean-field theory, and photoluminescence-based experiments. Our calculations establish CrPS$_4$ as a direct-gap semiconductor with a bandgap of 2.48~eV in the antiferromagnetic phase. Several sub-bandgap excitonic transitions are predicted by theory, comprising multiple spin-allowed excitons and an additional spin-flip excitation, predominantly localized on the Cr$^{3+}$ ions. Temperature- and magnetic-field-dependent optical measurements reveal thermally driven exciton redistribution among localized states and identify characteristic energy shifts that provide clear optical signatures of magnetic phase transitions in CrPS$_4$. These results provide new insights into the excitonic transitions of antiferromagnets and suggest potential routes for all-optical sensing and light-driven control of their magnetic order.

cond-mat.str-el↗

arXiv2026

Towards on-chip nascent all-van-der-Waals polarization optical components for nanoscale photonic applications

The integration of polarization-control elements into nanoscale photonic circuits remains a central challenge for modern on-chip optical technologies, which call for continuous miniaturization. Van der Waals (vdW) crystals provide a versatile platform for the creation of such components owing to their strong optical anisotropy, high-refractive indices and atomically precise heterostructure assembly capabilities. In this work, we demonstrate an approach towards the creation of all-vdW on-chip polarization optical components, exemplified with quarter-wave plates operating in the near-infrared (NIR) spectral region, realized in specifically twisted ReSe2/alpha-MoO3 vdW heterostructures on a Si/SiO2 platform. Here, low-symmetry ReSe2 layer serves as a source of exceptionally high linearly polarized excitonic emission, whereas in-plane birefringent alpha-MoO_3 provides polarization-state conversion. Furthermore, our finite-difference time-domain (FDTD) simulations quantitatively reproduce the experimental observations with high accuracy revealing the critical roles of layer thicknesses, twist-angle, Fabry-Perot interference and emitter distribution effects in the determination of polarization conversion efficiency, which yields up to 95 % degrees of circular polarization (DoCP) for the optimized parametrization. Our findings establish a practical route towards fully integrated all-vdW polarization optical components, providing a foundation for nanoscale photonic architectures based entirely on layered materials.

physics.optics↗

arXiv2026

Spin-flip optical excitations in van der Waals antiferromagnet CrPS$_4$

We investigate the near-infrared optical response of the semiconducting van der Waals antiferromagnet CrPS$_4$ and identify previously unreported spin-entangled optical resonances. The strong and anisotropic magnetic-field dependence of these resonances reflects the underlying magnetic order and confirms the biaxial antiferromagnetic nature of CrPS$_4$. From the magnetic field evolution of the optical transition, we extract key magnetic parameters, including the spin-flop ($\approx0.9$~T) and spin-saturation ($\approx8$~T) fields. These results demonstrate a potential pathway for all-optical probing of spin states in van der Waals antiferromagnets, with relevance for spin-sensitive optoelectronic and magneto-optical devices.

cond-mat.mtrl-sci↗

arXiv2026

Ferroelectric brightening of spin forbidden dark excitons in a WSe2/hybrid perovskite heterostructure

Long-lived dark excitons in monolayer WSe2 present promising candidates for carrying spin and valley information, but their optical access and spin manipulation have conventionally required the use of strong external magnetic fields. Here, using a ferroelectric hybrid perovskite heterostructure, we leverage the ferroelectric proximity effect to break the WSe2's in-plane rotational symmetry and brighten the spin-forbidden dark excitons under zero magnetic field conditions. Furthermore, we show that the twist angle between the WSe2 and perovskite crystals controls the ferroelectric coupling strength and valley-contrasting polarization. Our proposed mechanism, supported by a four-band tight-binding model, suggests that the ferroelectric proximity effect induces an asymmetric intersublattice interaction, generating an effective in-plane spin-orbit coupling (SOC) field that rotates spin/valley polarization and brightens dark excitons. Our work establishes ferroelectric proximity coupling as an electrically reconfigurable, magnetic-field-free strategy for spin exciton control in two-dimensional semiconductors.

cond-mat.mtrl-sci↗

arXiv2026

Generative design of inorganic materials

Materials discovery is fundamental to advance next-generation technologies as well as for sustainable and circular economy. Beyond computational screening, generative models are efficient at finding materials with desired properties, via multi-modal learning using multiscale data. This perspective examines the landscape of generative design for inorganic materials and discusses the integration of multi-modal learning with high-throughput experimental validation. We contextualize these challenges through the lens of a generative design framework as a unified approach to address the data-driven inverse design of functional materials. The central idea of the framework is constructed around a foundation AI model for inorganic materials interlinked deeply with various property databases and high-throughput experiments via a machine learning driven closed loop, which enables the framework to solve key challenges in functional materials. We argue that domain-specific implementations of such integrated workflows represent a promising pathway toward the unresolved challenge of data-driven inverse design for atom-engineered inorganic functional materials.

cond-mat.mtrl-sci↗

arXiv2026

Broadband dielectric permittivity tensor of muscovite for next-generation all van der Waals photonic components

We report a comprehensive determination of the broadband dielectric permittivity tensor of van der Waals (vdW) muscovite also referred to as mica, establishing it as a low-index low-loss platform for ultrathin nanophotonics. Resolving its anisotropic vibrational response and extracting accurate tensor components across broadband ultraviolet (UV) to near-infrared (NIR) spectral region, we show that vdW muscovite exhibits consistently low refractive indices negligible extinction and weak in-plane anisotropy allowing its effective treatment as a uniaxial dielectric in thin-film limits. Leveraging these properties, we design muscovite based vdW heterostructures pairing it MoS2, engineering few-layer distributed Bragg reflectors (DBR) and dichroic beam splitters (DBS) with high efficiency robust optical performance in a broad NIR spectral region achieved with sub-micron thicknesses. Our findings spotlight the high significance of low-index extinctionless vdW crystals, positioning muscovite as a highly perspective atomically flat building block for next-generation, broadband, all-vdW nanophotonic components.

physics.optics↗

arXiv2026

Polymer-free van der Waals assembly of 2D material heterostructures using muscovite crystals

The advent of van der Waals (vdW) heterostructures has enabled formation of bespoke materials with atomic precision, where numerous quantum and topological phenomena have already been discovered. This atomic-layer tunability, however, comes at a cost: individual 2D layers must be picked up, moved, and placed in a deterministic manner while keeping their interfaces atomically clean. Recent advances in machine learning and robotics place even stronger emphasis on the deterministic aspect of vdW assembly. Current polymer-based transfer methods satisfy neither the determinism nor cleanliness requirements. To this end, solutions are needed where adhesion can be dynamically and deterministically controlled without leaving organic contamination. Here, we present a polymer free transfer technique employing thin muscovite (mica) crystals. Temperature control over mica adhesion enables deterministic pick-up, stacking, and release of 2D materials, while their crystalline, inorganic nature ensures pristine interfaces and suppresses strain. Fully compatible with existing fabrication workflows, this approach enables the assembly of demanding vdW heterostructures, including those with exposed conductive layers, moiré superlattices and suspended membranes. Our method represents a promising strategy for vdW heterostructure fabrication toward its automatization.

cond-mat.mes-hall↗

arXiv2026

Surface defects in carbon-doped hexagonal boron nitride for negative-contrast direct laser writing

Radiative defects in hexagonal boron nitride (hBN) are active in a broad spectral range from deep ultraviolet to near-infrared wavelengths. Representatives of these defects act as bright single photon sources, spin-1 systems, and multiproperty atomic-scale sensors. They are predominantly investigated in bulk hBN films, where defects are decoupled from surface and interfacial effects. Here, we demonstrate a novel class of surface defects optically active in the green/yellow visible spectral range, which exhibit photophysical properties distinct from their bulk counterparts. High-power resonant laser illumination quenched the emission from the ensemble of such defects, which was attributed to a light-driven structural reconfiguration. The quenched defects were found to recover their emissive capabilities via a thermal cycling process, revealing an activation energy of 24.5 meV for the structural transition. Alternatively, permanent quenching of the defects was triggered by surface chemistry, involving lithiation-enabled attachment of functional groups. These mechanisms were utilized to realize negative-contrast direct laser writing, designing arbitrary geometric emissive patterns on demand in a microscopic configuration. The surface-active radiative centers in hBN appear particularly attractive for exploring environmental sensitivity, surface science, and coupling to photonic structures or electronic devices by taking unique advantage of the two-dimensional characteristics of the host lattice.

physics.optics↗

arXiv2026

Strong Spin-Lattice Interaction in Layered Antiferromagnetic CrCl$_\textrm{3}$

Understanding the coupling between lattice vibrations and magnetic order is crucial for controlling properties of two-dimensional magnetic materials. Here, we investigate the vibrational properties of bulk and thick-flake CrCl$_\textrm{3}$ using polarization-resolved Raman spectroscopy, complemented by photoluminescence, photoluminescence excitation, and optical absorption measurements. Symmetry analysis, supported by first-principles phonon calculations, enables the unambiguous assignment of all eight Raman-active modes, four $\textrm{A}_\textrm{g}$ and four $\textrm{E}_\textrm{g}$, previously predicted only theoretically. Excitation-energy-dependent measurements reveal that the strong enhancement of selected phonon modes originates primarily from interference effects rather than resonant Raman scattering. Temperature-dependent Raman spectroscopy further reveals pronounced signatures of spin-phonon coupling across the transition from a fully antiferromagnetic phase, through an intermediate regime with local, domain-like ferromagnetic order, to the paramagnetic phase, accompanied by a clear rhombohedral-to-monoclinic structural transition. Together, these results demonstrate how lattice, electronic, and magnetic degrees of freedom collectively govern the Raman response of CrCl$_\textrm{3}$.

cond-mat.mtrl-sci↗

arXiv2025

Deconstruction of the anisotropic magnetic interactions from spin-entangled optical excitations in van der Waals antiferromagnets

Magneto-optical excitations in antiferromagnetic d systems can originate from a multiplicity of light-spin and spin-spin interactions, as the light and spin degrees of freedom can be entangled. This is exemplified in van der Waals systems with attendant strong anisotropy between in-plane and out-of-plane directions, such as MnPS3 and NiPS3 films studied here. The rich interplay between the magnetic ordering and sub-bandgap optical transitions poses a challenge to resolve the mechanisms driving spin-entangled optical transitions, as well as the single-particle bandgap itself. Here we employ a high-fidelity ab initio theory to find a realistic estimation of the bandgap by elucidating the atom- and orbital-resolved contributions to the fundamental sub-bands. We further demonstrate that the spin-entangled excitations, observable as photoluminescence and absorption resonances, originate from an on-site spin-flip transition confined to a magnetic atom (Mn or Ni). The evolution of the spin-flip transition

cond-mat.mes-hall↗

arXiv2025

Electrically modulated light-emitting diodes driven by resonant and antiresonant tunneling between Cr$_2$Ge$_2$Te$_6$ electrodes

Exploring the electron tunneling mechanisms in diverse materials systems constitutes a versatile strategy for tailoring the properties of optoelectronic devices. In this domain, bipolar vertical tunneling junctions composed of van der Waals materials with vastly different electronic band structures enable simultaneous injection of electrons and holes into an optically active material, providing a universal blueprint for light-emitting diodes (LEDs). Efficient modulation of the injection efficiency has previously been demonstrated by creating resonant states within the energy barrier formed by the luminescent material. Here, we present an alternative approach towards resonant tunneling conditions by fabricating tunneling junctions composed entirely from gapped materials: Cr$_2$Ge$_2$Te$_6$ as electrodes, hBN as a tunneling barrier, and monolayer WSe$_2$ as a luminescent medium. The characterization of such LEDs revealed a nonmonotonous evolution of the electroluminescence intensity with the tunneling bias. The dominant role driving the characteristics of the electron tunneling was associated with the relative alignment of the density of states in Cr$_2$Ge$_2$Te$_6$ electrodes. The unique device architecture introduced here presents a universal pathway towards LEDs operating at room temperature with electrically modulated emission intensity.

cond-mat.mtrl-sci↗

arXiv2025

Two-dimensional materials as a multiproperty sensing platform

Two-dimensional (2D) materials have disrupted materials science due to the development of van der Waals technology. It enables the stacking of ultrathin layers of materials characterized by vastly different electronic structures to create man-made heterostructures and devices with rationally tailored properties, circumventing limitations of matching crystal structures, lattice constants, and geometry of constituent materials and supporting substrates. 2D materials exhibit extraordinary mechanical flexibility, strong light-matter interactions driven by their excitonic response, single photon emission from atomic centers, stable ferromagnetism in sub-nm thin films, fractional quantum Hall effect in high-quality devices, and chemoselectivity at ultrahigh surface-to-volume ratio. Consequently, van der Waals heterostructures with atomically flat interfaces demonstrate an unprecedented degree of intertwined mechanical, chemical, optoelectronic, and magnetic properties. This constitutes a foundation for multiproperty sensing, based on complex intra- and intermaterial interactions, and a robust response to external stimuli originating from the environment. Here, we review recent progress in the development of sensing applications with 2D materials, highlighting the areas where van der Waals heterostructures offer the highest sensitivity, simultaneous responses to multiple distinct externalities due to their atomic thickness in conjunction with unique material combinations, and conceptually new sensing methodology.

cond-mat.mes-hall↗

arXiv2025

Strong and selective magnon-phonon coupling in van der Waals antiferromagnet CoPS$_3$

The Raman scattering response of the biaxial antiferromagnet CoPS$_3$ has been investigated as a function of both magnetic field and temperature. The peaks observed in the low-frequency spectral range (90--200~cm$^{-1}$) have been identified as hybrid magnon--phonon excitations. The energies of the bare magnon and phonon modes, as well as the effective coupling strengths between different excitation pairs, have been determined. The strong and selective magnon--phonon interaction largely accounts for the pronounced splitting of two phonon-like modes observed at 152~cm$^{-1}$ and 158~cm$^{-1}$ in the antiferromagnetic phase of CoPS$_3$. Based on the identification of bare magnon excitations and their magnetic-field dependence, we propose an updated set of parameters for the effective exchange ($J_{\mathrm{eff}} = 9.9$~meV) and biaxial magnetic anisotropy ($D = 4.3$~meV and $E = -0.7$~meV) and advocate for an apparent anisotropic $g$-factor ($g_x = g_y = 2$, $g_z = 4$) in the CoPS$_3$ antiferromagnet.

cond-mat.mes-hall↗

arXiv2024

Unraveling the role of Ta in the phase transition of Pb(Ta1+xSe2)2 using low-temperature Raman spectroscopy

Phase engineering strategies in two-dimensional transition metal dichalcogenides (2D-TMDs) have garnered significant attention due to their potential applications in electronics, optoelectronics, and energy storage. Various methods, including direct synthesis, pressure control, and chemical doping, have been employed to manipulate structural transitions in 2D-TMDs. Metal intercalation emerges as an effective technique to modulate phase transition dynamics by inserting external atoms or ions between the layers of 2D-TMDs, altering their electronic structure and physical properties. Here, we investigate the significant structural phase transitions in Pb(Ta1+xSe2)2 single crystals induced by Ta intercalation using a combination of Raman spectroscopy and first-principles calculations. The results highlight the pivotal role of Ta atoms in driving these transitions and elucidate the interplay between intercalation, phase transitions, and resulting electronic and vibrational properties in 2D-TMDs. By focusing on Pb(Ta1+xSe2)2 as an ideal case study and investigating like metal intercalation, this study advances understanding in the field and paves the way for the development of novel applications for 2D-TMDs, offering insights into the potential of these materials for future technological advancements.

cond-mat.mtrl-sci↗

arXiv2023

Resonant Raman Scattering of Few Layers CrBr$_3$

We investigate the vibrational and magnetic properties of thin layers of chromium tribromide (CrBr$_3$) with a thickness ranging from three to twenty layers (3~L to 20~L) revealed by the Raman scattering (RS) technique. Systematic dependence of the RS process efficiency on the energy of the laser excitation is explored for four different excitation energies: 1.96 eV, 2.21 eV, 2.41 eV, and 3.06 eV. Our characterization demonstrates that for 12 L CrBr$_3$, 3.06~eV excitation could be considered resonant with interband electronic transitions due to the enhanced intensity of the Raman-active scattering resonances and the qualitative change in the Raman spectra. Polarization-resolved RS measurements for 12 L CrBr$_3$ and first-principles calculations allow us to identify five observable phonon modes characterized by distinct symmetries, classified as the A$_\textrm{g}$ and E$_\textrm{g}$ modes. The evolution of phonon modes with temperature for a 20 L CrBr$_3$ encapsulated in hexagonal boron nitride flakes demonstrates alterations of phonon energies and/or linewidths of resonances indicative of a transition between the paramagnetic and ferromagnetic state at Curie temperature ($T_\textrm{C} \approx 50$ K). The exploration of the effects of thickness on the phonon energies demonstrated small variations pronounces exclusively for the thinnest layers in the vicinity of 3 - 5 L. This observation is attributed to strong localization in the real space of interband electronic excitations, limiting the effects of confinement for resonantly excited Raman modes to atomically thin layers.

cond-mat.mtrl-sci↗

arXiv2023

Dielectric environment sensitivity of carbon centres in hexagonal boron nitride

A key advantage of utilizing van der Waals materials as defect-hosting platforms for quantum applications is the controllable proximity of the defect to the surface or the substrate for improved light extraction, enhanced coupling with photonic elements, or more sensitive metrology. However, this aspect results in a significant challenge for defect identification and characterization, as the defect's optoelectronic properties depend on the specifics of the atomic environment. Here we explore the mechanisms by which the environment can influence the properties of carbon impurity centres in hexagonal boron nitride (hBN). We compare the optical and electronic properties of such defects between bulk-like and few-layer films, showing alteration of the zero-phonon line energies, modifications to their phonon sidebands, and enhancements of their inhomogeneous broadenings. To disentangle the various mechanisms responsible for these changes, including the atomic structure, electronic wavefunctions, and dielectric screening environment of the defect center, we combine ab-initio calculations based on a density-functional theory with a quantum embedding approach. By studying a variety of carbon-based defects embedded in monolayer and bulk hBN, we demonstrate that the dominant effect of the change in the environment is the screening of the density-density Coulomb interactions within and between the defect orbitals. Our comparative analysis of the experimental and theoretical findings paves the way for improved identification of defects in low-dimensional materials and the development of atomic scale sensors of dielectric environments.

cond-mat.mtrl-sci↗

arXiv2023

Optical properties of orthorhombic germanium sulfide: Unveiling the Anisotropic Nature of Wannier Exciton

To fully explore exciton-based applications and improve their performance, it is essential to understand the exciton behavior in anisotropic materials. Here, we investigate the optical properties of anisotropic excitons in GeS encapsulated by h-BN, using different approaches that combine polarization- and temperature-dependent photoluminescence (PL) measurements, \textit{ab initio} calculations, and effective mass approximation (EMA). Using the Bethe-Salpeter Equation (BSE) method, we found that the optical absorption spectra in GeS are significantly affected by the Coulomb interaction included in the BSE method, which shows the importance of excitonic effects besides it exhibits a significant dependence on the direction of polarization, revealing the anisotropic nature of bulk GeS. Combining \textit{ab initio} calculations and EMA methods, we investigate the quasi-hydrogenic exciton states and oscillator strength (OS) of GeS along the zigzag and armchair axes. We found that the anisotropy induces lifting of the degeneracy and mixing of the excitonic states in GeS, which results in highly nonhydrogenic features. Very good agreement with the experiment is observed.

cond-mat.mes-hall↗

arXiv2023

Multidimensional sensing of proximity magnetic fields via intrinsic activation of dark excitons in WSe$_2$/CrCl$_3$ heterostructure

Quantum phenomena at interfaces create functionalities at the level of materials. Ferromagnetism in van der Waals systems with diverse arrangements of spins opened a pathway for utilizing proximity magnetic fields to activate properties of materials which would otherwise require external stimuli. Herewith, we realize this notion via creating heterostructures comprising bulk CrCl$_3$ ferromagnet with in-plane easy-axis magnetization and monolayer WSe$_2$ semiconductor. We demonstrate that the in-plane component of the proximity field activates the dark excitons within WSe$_2$. Zero-external-field emission from the dark states allowed us to establish the in-plane and out-of-plane components of the proximity field via inspection of the emission intensity and Zeeman effect, yielding canted orientations at the degree range of $10^{\circ}$ $-$ $30^{\circ}$ at different locations of the heterostructures, attributed to the features of interfacial topography. Our findings are relevant for the development of spintronics and valleytronics with long-lived dark states in technological timescales and sensing applications of local magnetic fields realized simultaneously in multiple dimensions.

cond-mat.mes-hall↗