arXiv subjects

Maciej R. Molas

Publications and source records attributed to Maciej R. Molas.

At least 19 recordsLinked to original sources

arXiv2026

Spin-phonon coupling and isotope-related pseudo-molecule vibrations in layered Cr$_2$Ge$_2$Te$_6$ ferromagnet

The vibrational structure of chromium germanium telluride (Cr$_2$Ge$_2$Te$_6$, CGT) is investigated and a strong spin-phonon coupling is revealed. The measured high-resolution Raman scattering (RS) spectra are composed of the 10 Raman-active modes: 5A$_\textrm{g}$ and 5E$_\textrm{g}$, predicted by calculation using the density functional theory and identified using polarization-resolved RS measurements. We also studied the effect of temperature on the RS spectra of CGT from 5~K to 300~K. A strong magneto-phonon coupling in CGT is revealed at temperatures of about 150~K and 60~K, which are associated with the appearance of the local magnetic order in the material and the transition to the complete ferromagnetic phase, respectively. Moreover, a unique shape of the A$_g^5$ mode composed of a set of very narrow Raman peaks is simulated using a model that takes into account vibrations of Ge-Ge pseudo-molecules for various Ge isotopes.

cond-mat.mtrl-sci↗

arXiv2026

Ultralow-Tensile Strain Enables Exciton Funneling and Energy Transfer to Boost MoSe2 Photoluminescence Quantum Yield

Strain engineering is a powerful route for controlling the exciton dynamics in van der Waals (vdW) heterostructures (HSs). The interlayer energy transfer (ET) process is another key factor in controlling the photocarrier relaxation pathways in vdW HSs. In this work, we combine these two processes to achieve an 8-fold enhancement to the relative photoluminescence (PL) quantum yield (QY) in a HS formed from monolayers of ReS2 and MoSe2, separated by a thin hBN interlayer, placed onto an hBN bubble. We achieve this enhancement by applying only 0.1% biaxial tensile strain, which results in efficient exciton funneling and an increased transition dipole moment. Our experimental data are supported by first-principles density-functional theory and coherent transfer-matrix method calculations, ruling out optical interference as the dominant origin of the enhancement. This work provides an innovative route for enhancing the PL QY of vdW materials via interplay between the tensile strain and the ET process.

cond-mat.mtrl-sci↗

arXiv2026

Layer-Dependent Vibrational and Optical Properties of $\mathrm{Mo}{0.58}\mathrm{W}{0.42}\mathrm{Se}_2$ Alloy

Semiconducting Mo$_x$W$_{1-x}$Se$_2$ alloys provide a versatile platform for tailoring the optical properties of two-dimensional materials through both composition and layer thickness. Here, we systematically investigate mechanically exfoliated Mo$_{0.58}$W$_{0.42}$Se$_2$ flakes ranging from monolayer (1L) to nine layers by combining Raman scattering (RS), photoluminescence (PL), reflectance contrast (RC) spectroscopy, and first-principles phonon calculations. Thirteen RS peaks are identified, including the low-frequency interlayer shear mode, whose thickness dependence is well described by a linear-chain model, yielding an interlayer force constant of $K_s=(2.996\pm0.015)\times10^{19}$ N m$^{-3}$. PL measurements reveal a crossover from the direct-bandgap 1L to indirect-bandgap multilayers. The thickness evolution of the indirect optical transition is quantitatively reproduced using a quantum-confinement model, yielding an out-of-plane reduced effective mass of $μ_\perp=0.75 m_0$. RC spectroscopy reveals four excitonic resonances. While the A and B excitons associated with the $K^\pm$ valleys remain nearly independent of layer thickness, the higher-energy C and D resonances originating from the band-nesting regions exhibit pronounced redshifts, reflecting substantial thickness-induced modifications of the electronic band structure. These results establish comprehensive spectroscopic fingerprints of flake thickness, interlayer coupling, and electronic structure in Mo$_x$W$_{1-x}$Se$_2$ alloys and provide a reliable, non-destructive framework for their optical characterization.

cond-mat.mes-hall↗

arXiv2026

Metallic-Phase-Fe$_3$GaTe$_2$ Enabled Interface Engineering for Self-Powered and High-Gain WS$_2$ Photodetectors

Two-dimensional transition-metal dichalcogenides offer strong light-matter interaction but suffer from inefficient carrier separation and contact-related losses in photodetectors. Here, we demonstrate a high-gain WS$_2$/Fe$_3$GaTe$_2$ van der Waals heterostructure photodetector, where metallic Fe$_3$GaTe$_2$ serves as an active interfacial contact. The work-function mismatch, together with interfacial charge redistribution and asymmetric contact geometry, contributes to a built-in field that supports self-powered photodetection at zero bias. Under 450 nm illumination, the device delivers a zero-bias responsivity of 23.5 A/W and an apparent external quantum efficiency of 6.4 x 10$^3$%. At -1 V biasing, the heterostructure exhibits photoresponse at 450, 520 and 633 nm, achieving a responsivity of 9.7 x 10$^3$ A/W and a noise derived specific detectivity of 2.3 x 10$^13$ Jones at 100 Hz under 450 nm illumination. The high photoresponse is attributed to interfacial carrier separation, efficient extraction, and a likely contribution from trap-assisted photogating in multilayer WS$_2$. These results establish Fe$_3$GaTe$_2$-enabled interface engineering as an effective route for self-powered, highly sensitive 2D photodetectors.

cond-mat.mtrl-sci↗

arXiv2026

Layer-Dependent Phonons, Excitons, and Magneto-Optical Phenomena in CrSBr: A Mini Review

Two-dimensional layered magnetic materials offer a versatile platform for exploring low-dimensional magnetism and coupled many-body interactions in these materials. Chromium sulfur bromide (CrSBr) is a promising candidate for advanced spintronic and optoelectronic applications because of its intrinsic air stability, semiconducting nature, strong in-plane anisotropy, and A-type antiferromagnetic ordering. This review summarizes recent advances in the understanding of the layer-dependent vibrational and excitonic properties of CrSBr, as well as its magneto-optical response, from bulk crystals to the monolayer limit. We examined its crystal structure, magnetic anisotropy, and interlayer spin reorientation, followed by insights into vibrational dynamics and spin-phonon coupling. Particular emphasis is placed on the excitonic landscape, including magnetic-field-sensitive photoluminescence, localized excitonic states, and the coexistence of Frenkel- and Wannier-Mott excitons in the bandgap. Finally, we discuss the challenges and prospects of harnessing the unique layer-dependent properties of CrSBr in spintronic, magneto-optical, and quantum photonic technologies.

cond-mat.mes-hall↗

arXiv2026

Chiral Phonons and Giant Anisotropic Photoresponse in Quasi-1D van der Waals Semiconductor ZrSnS3

Low-dimensional van der Waals semiconductors with reduced symmetry provide a unique platform for exploring anisotropic physical properties. The quasi-one-dimensional family MXQ$_3$ (M = Hf, Zr; X = Sn; Q = S, Se) exhibits notable structural anisotropy, where zigzag atomic chains influence optical phenomena such as birefringence. This study investigates anisotropic lattice dynamics in ZrSnS$_3$ using angle- and polarization-dependent Raman spectroscopy. Temperature-dependent measurements reveal anharmonic phonon behavior, indicating strong phonon-phonon coupling. Density functional theory calculations show good agreement with the experimentally observed Raman spectra, validating the microscopic description of the lattice dynamics. We also observe a helicity-dependent intensity and a reversal in phonon intensity between lower- and higher-frequency modes under circularly polarized light, which is characteristic of chiral phonons governed by the polarization of the Zr/Sn chains. Our first-principles analysis further shows that angular-momentum-like phonon textures can emerge away from the $Γ$-point near mode-hybridization and avoided-crossing regions, providing microscopic insight into the observed helicity-dependent Raman signatures. Furthermore, we fabricate an optoelectronic device from a thin ZrSnS$_3$ nanowire, demonstrating a photoresponsivity of 50~mA/W under 520~nm laser excitation (1~mW/cm$^2$). The device exhibits a pronounced, power-scalable anisotropic photoresponse with a clear preferred polarization direction. These results highlight the coupling mechanisms between polarization, lattice vibrations, and charge carriers in ZrSnS$_3$, establishing it as a promising material for polarization-sensitive optoelectronics and directional quantum transport.

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↗

arXiv2026

Dopant-induced modifications of the optical properties of GaSe

Doping plays a crucial role in tailoring the electronic, optical, and magnetic properties of semiconductors, enabling control of carrier dynamics and the formation of functional states for optoelectronic applications. We investigate the influence of Fe dopants on the optical properties of GaSe crystals using photoluminescence (PL) spectroscopy under varying excitation power, temperature, and magnetic field. Fe incorporation introduces multiple sharp emission lines in addition to intrinsic excitonic transitions, including free and localised excitons. Power- and temperature-dependent measurements indicate that these emission features are associated with Fe-related dopant centres (Fe-bound excitons). Magneto-PL measurements reveal two distinct families of $g$-factors, enabling the identification of intrinsic excitonic transitions and Fe-induced defect states. These results demonstrate that Fe doping creates optically and magnetically active centres in GaSe, providing insight into defect-related excitonic processes and their potential relevance for magneto-optoelectronic and quantum photonic applications.

cond-mat.mtrl-sci↗

arXiv2026

Resonant Raman scattering in bilayer 3R-MoS$_{2}$

Raman scattering is a powerful spectroscopic technique widely employed to investigate light-matter interactions and lattice dynamics in two-dimensional materials. Here, we investigate the temperature-dependent resonant Raman response of bilayer 3R-MoS$_2$. The study combines multi-wavelength Raman spectroscopy, photoluminescence measurements, and density functional theory calculations to track the evolution of excitonic transitions and resonance conditions. We observe contributions from both zone-centre and finite-momentum phonons, a pronounced quenching of the Stokes intensity at low temperatures followed by saturation, the emergence of anti-Stokes scattering above 130~K, and a strong deviation of the effective phonon temperature from the lattice temperature induced by resonance effects. These results demonstrate that the Raman response is governed by the interplay between incoming and outgoing resonance processes, providing deeper insight into exciton-phonon coupling in van der Waals materials.

cond-mat.mtrl-sci↗

arXiv2026

Doping-Induced Brightening of Dark Excitons and Trions in a WSe$_2$ Monolayer

Optically dark excitonic states play a critical role in the valleytronic, electronic, and optical properties of monolayer semiconducting transition metal dichalcogenides. Here, we investigate how electrostatic doping affects the in-plane magnetic-field-induced activation of dark excitonic complexes in a gated WSe$_2$ monolayer. By continuously tuning the carrier density via gate voltage, we access $n$-type, charge-neutral, and $p$-type regimes and track the corresponding brightening dynamics. We find that the brightening rates of the dark negative trion ($T^{D-}$), dark neutral exciton ($X^{D}$), and dark positive trion ($T^{D+}$) exhibit a strong and nontrivial dependence on doping. In particular, the pronounced asymmetry in the brightening behaviour of the neutral $X^{D}$ complex and the charged $T^{D-}$ and $T^{D+}$ trions reveals distinct underlying carrier interactions, which we describe using a rate-equation model for their steady-state populations. These findings highlight the key role of dark excitonic complexes in governing the optical response and carrier dynamics of doped S-TMD monolayers.

cond-mat.mes-hall↗

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↗

arXiv2026

Raman scattering fingerprints of the charge density wave state in one-dimensional NbTe$_4$

Charge-density waves (CDWs) are ordered quantum states of conduction electrons accompanied by periodic lattice distortions. Raman scattering (RS) spectroscopy is therefore well suited for probing CDW-induced structural modulations. We investigate the CDW state in quasi-one-dimensional NbTe$_4$ using RS spectroscopy. At $T$=5~K, the resonantly enhanced Raman spectrum exhibits 25 phonon modes. Polarization-dependent measurements reveal a strong coupling between phonon-mode symmetry and crystallographic symmetry, with modes polarized parallel or perpendicular to the crystallographic $c$-axis, along which the one-dimensional structure is elongated. Temperature-dependent RS measurements identify a transition between commensurate and incommensurate CDW phases, accompanied by pronounced thermal hysteresis, with transition temperatures of approximately 45~K upon cooling and 90~K upon warming. The hysteresis width depends on the warming rate, indicating a finite nucleation rate of CDW domains and suggesting potential relevance for memory-device applications.

cond-mat.mtrl-sci↗

arXiv2025

Fast Interlayer Energy Transfer from the Lower Bandgap MoS2 to the Higher Bandgap WS2

Energy transfer (ET) is a dipole-dipole interaction, mediated by the virtual photon. Traditionally, ET happens from the higher (donor) to lower bandgap (acceptor) material. However, in some rare instances, ET can happen from the lower-to-higher bandgap material, depending on the strong overlap between the acceptor photoluminescence (PL) and the donor absorption spectra. In this work, we report an ET process from the lower bandgap MoS2 to the higher bandgap WS2, due to a near 'resonant' overlap between the MoS2 B and WS2 A excitonic levels. Changing the MoS2 bandgap from direct-to-indirect by increasing the layer number results in a reduced ET rate, evidenced by the quenching of the WS2 PL emission. Our work shows at 300 K, the ET timescale of ~33 fs is faster than the reported thermalization of the MoS2 excitonic intervalley scattering (K to K') time and competing with the ultrafast charge transfer timescale. Thus, allowing us to open a new direction in understanding the competing inter/intralayer processes.

cond-mat.mtrl-sci↗

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

Extremely high excitonic $g$-factors in 2D crystals by alloy-induced admixing of band states

Monolayers (MLs) of semiconducting transition metal dichalcogenides (\mbox{S-TMDs}) emit light very efficiently and display rich spin-valley physics, with gyromagnetic ($g$-) factors of about -4. Here, we investigate how these properties can be tailored by alloying. Magneto-optical spectroscopy is used to reveal the peculiar properties of excitonic complexes in Mo$_{x}$W$_{1-x}$Se$_2$ MLs with different Mo and W concentrations. We show that the alloys feature extremely high $g$-factors for neutral excitons, that change gradually with the composition up to reaching values of the order of -10 for $x \approx 0.2$. First-principles calculations corroborate the experimental findings and provide evidence that alloying in S-TMDs results in a non-trivial band structure engineering, being at the origin of the high $g$-factors. The theoretical framework also suggests a higher strain sensitivity of the alloys, making them promising candidates for tailor-made optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Magneto-Excitonic Duality From Monolayer to Trilayer CrSBr

Two-dimensional (2D) layered magnetic materials (LMMs) are a newly emerging class of van der Waals materials, opening new opportunities to study magneto-excitonic coupling. The air-stable, structurally and optically anisotropic A-type antiferromagnetic chromium sulfur bromide (CrSBr) is one of the most prominent examples of such LMMs. We investigate photoluminescence (PL) and PL excitation of mono- to tri-layers CrSBr and find that it exhibits a unique duplexity, supporting both Frenkel- and Wannier-Mott-like excitons. Our magneto-optical experiments reveal a similar excitonic response from the mono- and trilayer systems and a completely different signature in the bilayer flake. This shows a different origin of the low-lying excitonic species (A, A', and B) in the band structure. We confirm the robustness of the magneto-excitonic coupling in few-layer CrSBr. Our work enables a more comprehensive exploration of the dual excitonic behavior in 2D materials.

cond-mat.mtrl-sci↗

arXiv2024

Pressure-induced optical anisotropy of HfS$_2$

The effect of pressure on Raman scattering (RS) in the bulk HfS$_2$ is investigated under hydrostatic and non-hydrostatic conditions. The RS lineshape does not change significantly in the hydrostatic regime, showing a systematic blueshift of the spectral features. In a non-hydrostatic environment, seven peaks emerge in the spectrum ($P$=7 GPa) dominating the lineshape up to $P$=10.5 GPa. The change in the RS lineshape manifests a pressure-induced phase transition in HfS$_2$. The simultaneous observation of both low-pressure (LP) and high-pressure (HP) related RS peaks suggests the corresponding coexistence of two different phases over a large pressure range. We found that the HP-related phase is metastable, persisting during the decompression cycle down to $P$=1.2 GPa with the LP-related features finally recovering at even lower pressures. The angle-resolved polarized RS (ARPRS) performed under $P$=7.4 GPa revealed a strong in-plane anisotropy of both the LP-related A$_{1g}$ mode and the HP peaks. The anisotropy is related to the possible distortion of the structure induced by the non-hydrostatic component of the pressure. We describe the obtained results by the influence of the non-hydrostatic pressure on the observed phase transition. We interpret our results in terms of a distorted $Pnma$ phase as a possible HP induced structure of HfS$_2$.

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↗