arXiv subjects

Otakar Frank

Publications and source records attributed to Otakar Frank.

At least 19 recordsLinked to original sources

arXiv2026

Three-dimensional excitonic dipole anisotropy enables ultrabroadband polarization photodetection in CrCl3

Simultaneous detection of the spectral and polarization properties of light is highly desirable for integrated imaging and photonic technologies but typically requires complex multi-component architectures. Here, we demonstrate that the intrinsic dielectric anisotropy of layered insulating CrCl3 enables ultrabroadband polarization-resolved photodetection spanning wavelengths from 300 to 1700 nm. The photoresponse is governed by long-lived ligand-field excitons, whose microsecond-scale lifetime produces a photoconductive gain exceeding 4.5 x 10^4. By combining wavelength-, polarization-, and angle-resolved optoelectronic measurements, we reveal that distinct ligand-field and higher-energy excitonic transitions possess different optical dipole orientations, leading to excitation-energy-dependent rotation of the in-plane polarization axis. Furthermore, oblique illumination activates out-of-plane optical dipoles, while competing excitonic transitions with distinct dipole orientations drive wavelength-dependent rotation and reversal of the polarization anisotropy. Together, these effects produce a highly tunable degree of polarization ranging from -90% to +75%, establishing intrinsic three-dimensional vectorial light-matter interactions in a layered magnetic van der Waals insulator. These findings establish dielectric anisotropy and excitonic dipole engineering as powerful design principles for compact ultrabroadband polarization-sensitive photodetectors and multifunctional van der Waals photonic systems.

physics.optics↗

arXiv2026

Interplay of Cl Substitution and He$^{+}$ Irradiation in CrSBr$_{1-x}$Cl$_{x}$

Two-dimensional magnetic semiconductors provide a promising platform for exploring the interplay between disorder, lattice dynamics, and resonant light--matter interactions. Among them, CrSBr exhibits strong in-plane anisotropy and pronounced resonance-enhanced Raman scattering. Here, we investigate the effects of Cl substitution and He$^{+}$ irradiation on the vibrational response of CrSBr using polarization-resolved Raman spectroscopy. Cl substitution activates additional phonon modes associated with local symmetry breaking, while He$^{+}$ irradiation introduces distinct defect-related scattering channels and enhanced phonon broadening. The combined effects of alloy disorder and externally introduced defects lead to strong anisotropic reconstruction of the Raman spectra and modification of the nonlinear Raman response under near-resonant 1.96 eV excitation. Power-dependent measurements reveal robust superlinear scaling of both intrinsic and substitution-induced phonon modes, indicating persistent resonance-enhanced electron--phonon coupling even in defect-engineered samples.

cond-mat.mes-hall↗

arXiv2026

The Topography Trap: Sifting Interlayer Excitons from Strain-Related Artifacts in Real-World 2D Hetrostructures

Novel excitonic phenomena emerging in transition metal dichalcogenide (TMDC) heterostructures belong to the most exciting topics in contemporary physics of van der Waals materials. Interlayer excitons (IXs) stand out among those due to their long radiative lifetimes and tunability by electric fields, strain, and twist angle. However, many ambiguities persist in the optical identification and manipulation of IXs, highlighting the need for reliable spectroscopic criteria that distinguish interlayer species from spurious signals. Here, we present a decision-tree protocol that evaluates interlayer coupling via intralayer exciton quenching and correlates photoluminescence (PL) with atomic force microscopy (AFM) to correctly assign room-temperature PL features in TMDC-based heterostructures. Applying this protocol, we identify momentum-direct IX between the K valleys of the two layers (KK-IX) in MoS2-MoSe2 and MoS2-WSe2 heterostructures at room temperature. In contrast, our protocol contests the reported bright, momentum-indirect, twist-angle-independent $Γ$K-IX in MoS2-WSe2. Comprehensive experimental data, including infrared and tip-enhanced photoluminescence (TEPL) with sub-diffraction-limited resolution, show no compelling evidence for this excitonic species, despite numerous reports. Instead, the spectroscopic features previously assigned to this $Γ$K-IX originate from locally strained WSe2 at topographical inhomogeneities of the heterostructure interface, underscoring the need for robust, spatially resolved characterization of real-world samples in this highly accessible field and providing a generally applicable framework for identifying interlayer excitons in 2D semiconductor heterostructures.

cond-mat.mes-hall↗

arXiv2026

Robust phonon engineering and symmetry-selective lattice dynamics in CrSBr$_{1-x}$Cl$_{x}$

Atomic substitution provides a controlled route to engineer lattice dynamics in low-symmetry two-dimensional materials. Here, by combining polarization-resolved Raman spectroscopy and first-principles calculations, we investigate the evolution of phonon characteristics in CrSBr$_{1-x}$Cl$_{x}$ ($0 \leq x \leq \sim 0.5$) upon partial substitution of Br with Cl atoms. Progressive Cl substitution of Br induces systematic shifts of parent CrSBr out-of-plane $A_\textrm{g}$ phonon modes and activates additional Raman features. These features persist across different polarization configurations and excitation energies, reflecting substitution-induced symmetry lowering and local lattice perturbations. Explicit supercell phonon calculations combined with Raman $Γ$-density-of-states simulations identify these features as symmetry-lowered descendants of parent modes arising from alloy disorder. Complementary strain-dependent calculations reveal that anisotropic lattice compression plays a key role in renormalizing Cr-S dominated phonons. Under near-resonant excitation, stimulated Raman scattering-like amplification remains observable with increasing Cl content, highlighting the resilience of anisotropic electron-phonon coupling in this system.

cond-mat.mtrl-sci↗

arXiv2025

Resonance Raman Scattering and Anomalous Anti-Stokes Phenomena in CrSBr

CrSBr, a van der Waals material, stands out as an air-stable magnetic semiconductor with appealing intrinsic properties such as crystalline anisotropy, quasi-1D electronic characteristics, layer-dependent antiferromagnetism, and non-linear optical effects. In this study, we investigate the differences between the absorption and emission spectra, focusing on the origin of the emission peak near 1.7 eV observed in the photoluminescence spectrum of CrSBr. Our findings are corroborated by excitation-dependent Raman experiments. Additionally, we explore the anti-Stokes Raman spectra and observe an anomalously high anti-Stokes to Stokes intensity ratio of up to 0.8, which varies significantly with excitation laser power and crystallographic orientation relative to the polarization of the scattered light. This ratio is notably higher than that observed in graphene ($\approx$ 0.1) and MoS$_2$ ($\approx$ 0.4), highlighting the unique vibrational and electronic interactions in CrSBr. Lastly, we examine stimulated Raman scattering and calculate the Raman gain in CrSBr, which attains a value of 1 $\times$ 10$^{8}$ cm/GW, nearly four orders of magnitude higher than that of previously studied three-dimensional systems.

cond-mat.mes-hall↗

arXiv2024

Strain-Induced Decoupling Drives Gold-Assisted Exfoliation of Large-Area Monolayer 2D Crystals

Gold assisted exfoliation (GAE) is a groundbreaking mechanical exfoliation technique, producing centimeter scale single crystal monolayers of 2D materials. Such large, high quality films offer unparalleled advantages over the micron sized flakes typically produced by conventional exfoliation techniques, significantly accelerating the research and technological advancements in the field of 2D materials. Despite its wide applications, the fundamental mechanism of GAE remains poorly understood. In this study, using MoS2 on Au as a model system, we employ ultralow frequency Raman spectroscopy to elucidate how the interlayer interactions within MoS2 crystals are impacted by the gold substrate. The results reveal that the coupling at the first interface between the adhered layer on the gold substrate and the adjacent layer, is substantially weakened, with the binding force being reduced to nearly zero. This renders the first interface the weakest point in the system, thereby the crystal preferentially cleaves at this junction, generating large area monolayers with sizes comparable to the parent crystal. Biaxial strain in the adhered layer, induced by the gold substrate, is identified as the driving factor for the decoupling effect. We establish the strain-induced decoupling effect as the primary mechanism of GAE, which could also play a significant role in general mechanical exfoliations.

cond-mat.mtrl-sci↗

arXiv2021

Probing the Local Dielectric Function by Near Field Optical Microscopy Operating in the Visible Spectral Range

The optoelectronic properties of nanoscale systems such as carbon nanotubes (CNTs), graphene nanoribbons and transition metal dichalcogenides (TMDCs) are determined by their dielectric function. This complex, frequency dependent function is affected by excitonic resonances, charge transfer effects, doping, sample stress and strain, and surface roughness. Knowledge of the dielectric function grants access to a material's transmissive and absorptive characteristics. Here we introduce the dual scanning near field optical microscope (dual s-SNOM) for imaging local dielectric variations and extracting dielectric function values using a mathematical inversion method. To demonstrate our approach, we studied a monolayer of WS$_2$ on bulk Au and identified two areas with differing levels of charge transfer. Our measurements are corroborated by atomic force microscopy (AFM), Kelvin force probe microscopy (KPFM), photoluminescence (PL) intensity mapping, and tip enhanced photoluminescence (TEPL). We extracted local dielectric variations from s-SNOM images and confirmed the reliability of the obtained values with spectroscopic imaging ellipsometry (SIE) measurements.

cond-mat.mtrl-sci↗

arXiv2021

Addressing Raman features of individual layers in isotopically labeled Bernal stacked bilayer graphene

The most important bands for the evaluation of strain in graphene (the 2D and 2D prime modes) are investigated. It is shown that for Bernal-stacked bilayers, the two-phonon Raman features have three different components that can be assigned to processes originating solely from the top graphene layer, bottom graphene layer, and from a combination of processes originating both from the top and bottom layers. The individual components of the 2D and 2D prime modes are disentangled. The reported results enable addressing the properties of individual graphene layers in isotopically labelled turbostratic and Bernalstacked graphene systems.

cond-mat.mtrl-sci↗

arXiv2021

Temperature and Face Dependent Copper-Graphene Interactions

The interaction between graphene and metals represents an important issue for the large-area preparation of graphene, graphene transfer and the contact quality in graphene devices. We demonstrate a simple method for estimating and manipulating the level of interaction between graphene and copper single crystals through heat treatment, at temperatures from 298K to 1073K. We performed an in-situ Raman spectroscopy showing Cu face-specific behavior of the overlying graphene during the heat treatment. On Cu(111) the interaction is consistent with theoretical predictions and remains stable, whereas on Cu(100) and Cu(110), the initially very weak interaction and charge transfer can be tuned by heating. Our results also suggest that graphene grown on Cu(100) and Cu(110) is detached from the copper substrate, thereby possibly enabling an easier graphene transfer process as compared to Cu (111).

cond-mat.mtrl-sci↗

arXiv2021

Effect of layer number and layer stacking registry on the formation and quantification of defects in graphene

Correct defect quantification in graphene samples is crucial both for fundamental and applied re-search. Raman spectroscopy represents the most widely used tool to identify defects in graphene. However, despite its extreme importance the relation between the Raman features and the amount of defects in multilayered graphene samples has not been experimentally verified. In this study we intentionally created defects in single layer graphene, turbostratic bilayer graphene and Bernal stacked bilayer graphene by oxygen plasma. By employing isotopic labelling, our study reveals substantial differences of the effects of plasma treatment on individual layers in bilayer graphene with different stacking orders. In addition Raman spectroscopy evidences scattering of phonons in the bottom layer by defects in the top layer for Bernal-stacked samples, which can in general lead to overestimation of the number of defects by as much as a factor of two.

cond-mat.mtrl-sci↗

arXiv2020

Imaging Nanoscale Inhomogeneities and Edge Delamination in As-Grown MoS2 Using Tip-Enhanced Photoluminescence

Methods for nanoscale material characterization are in ever-increasing demand, especially those that can provide a broader range of information at once. Near-field techniques based on combinations of scanning probe microscopy (SPM) and Raman or photoluminescence (PL) spectroscopy (tip-enhanced Raman spectroscopy [TERS] and/or tip-enhanced photoluminescence [TEPL]) are, thanks to their capabilities and fast development, strong candidates for becoming widespread across the scientific community as SPM and Raman microscopy did only a decade or two ago. Herein, a gap-less TEPL study is performed directly on as-grown MoS2 monolayer samples without any pretreatment or transfer, i.e., without the utilization of plasmonic substrate. Thanks to a mapping resolution as low as a few tens of nanometers, homogeneous layer interiors from defective edge fronts in the grown monolayers can be distinguished. With the aid of additional high-resolution SPM modes, like local surface potential and capacitance measurements, together with nanomechanical mapping, a combination of defects and a lack of substrate doping is suggested as being responsible for the observed PL behavior in the partially delaminated MoS2 layers. In contrast, mechanically exfoliated flakes show topography- and contamination-related heterogeneities in the whole flake area.

physics.app-ph↗

arXiv2020

Strong Localization Effects in the Photoluminescence of Transition Metal Dichalcogenide Heterobilayers

The emergence of various exciton-related effects in transition metal dichalcogenides (TMDC) and their heterostructures has inspired a significant number of studies and brought forth several possible applications. Often, standard photoluminescence (PL) with microscale lateral resolution is utilized to identify and characterize these excitonic phenomena, including interlayer excitons (IEXs). We studied the local PL signatures of van der Waals heterobilayers composed of exfoliated monolayers of the (Mo,W)(S,Se)$_2$ TMDC family with high spatial resolution (down to 30 nm) using tip-enhanced photoluminescence (TEPL) with different orders (top/bottom) and on different substrates. We evidence that other PL signals may appear near the reported energy of the IEX transitions, possibly interfering in the interpretation of the results. While we can distinguish and confirm the presence of IEX-related PL in MoS$_2$-WS$_2$ and MoSe$_2$-WSe$_2$, we find no such feature in the MoS$_2$-WSe$_2$ heterobilayer in the spectral region of 1.7-1.4 eV, where the IEXs of this heterobilayer is often reported. We assign the extra signals to the PL of the individual monolayers, in which the exciton energy is altered by the local strains caused by the formation of blisters and nanobubbles, and the PL is extremely enhanced due to the decoupling of the layers. We prove that even a single nanobubble as small as 60 nm---hence not optically visible---can induce such a suspicious PL feature in the micro-PL spectrum of an otherwise flat heterobilayer.

cond-mat.mes-hall↗

arXiv2020

Fingerprints of the Strong Interaction between Monolayer MoS2 and Gold

Gold-mediated exfoliation of MoS2 has attracted considerable interest in the recent years. A strong interaction between MoS2 and Au facilitates preferential production of centimeter-sized monolayer MoS2 with near-unity yield and provides a heterostructure system noteworthy from a fundamental standpoint. However, little is known about the detailed nature of the MoS2-Au interaction and its evolution with the MoS2 thickness. Here, we identify specific vibrational and binding energy fingerprints of such strong interaction using Raman and X-ray photoelectron spectroscopy, which indicate substantial strain and charge-transfer in monolayer MoS2. Near-field tip-enhanced Raman spectroscopy reveals heterogeneity of the MoS2-Au interaction at the nanoscale, reflecting the spatial non-conformity between the two materials. Far-field micro-Raman spectroscopy shows that this interaction is strongly affected by the roughness and cleanliness of the underlying Au. Our results elucidate the nature of the strong MoS2-Au interaction and provide guidance for strain and charge doping engineering of MoS2.

cond-mat.mtrl-sci↗

arXiv2018

Graphene under direct compression: stress effects and interlayer coupling

In this work we explore mechanical properties of graphene samples of variable thickness. For this purpose, we coupled a high pressure sapphire anvil cell to a micro-Raman spectrometer. From the evolution of the G band frequency with stress we document the importance the substrate has on the mechanical response of graphene. On the other hand, the appearance of disorder as a conse-quence of the stress treatment has a negligible effect on the high stress behaviour of graphene.

cond-mat.mtrl-sci↗

arXiv2018

Strain Assessment in Graphene Through the Raman 2D' Mode

Accurate and simple local strain assessment in graphene is one of the crucial tasks in device characterization. Raman spectroscopy is often used for that purpose through monitoring of the G and 2D modes. However, the shifts of those two bands might be biased, especially under uniaxial strain, by the effects of charge-transfer doping. Therefore, it is extremely desirable to use another Raman band, less affected by doping, but with a defined and measurable behavior under strain. The Raman 2D' mode is in this sense the ideal feature for the evaluation of strain levels in stretched graphene monolayers, suitable for this task even under different experimental conditions. The sensitivity and accuracy of the approach through 2D' mode is on the same level as through the G mode, however, the clear advantage of the 2D' arises when doping effects are present in the sample.

cond-mat.mtrl-sci↗

arXiv2018

Raman spectroscopy and In-situ Raman spectroelectrochemistry of isotopically engineered graphene systems

The unique properties of graphene offer immense opportunities for applications to many scientific fields, as well as societal needs, beyond our present imagination. One of the important features of graphene is the relatively simple tunability of its electronic structure, an asset which extends the usability of graphene even further beyond present experience. A direct injection of charge carriers into the conduction or valence bands, i.e., doping, represents a viable way of shifting the Fermi level. In particular, the electrochemical doping should be the method of choice, when higher doping levels are desired and when a firm control of experimental conditions is needed. In this Account, we focus on the electrochemistry of graphene in combination with in-situ Raman spectroscopy, i.e., the in-situ Raman spectroelectrochemistry. Such a combination of methods is indeed very powerful, since Raman spectroscopy can readily monitor not only the changes in the doping level, but it can give information also on eventual stress or disorder in the material. However, when employing Raman spectroscopy, one of its main strengths lies in the utilization of isotope engineering during the chemical vapor deposition (CVD) growth of the graphene samples. The in-situ Raman spectroelectrochemical study of multi-layered systems with smartly designed isotope compositions in individual layers can provide a plethora of knowledge about the mutual interactions: (i) between the graphene layers themselves, (ii) between graphene layers and their directly adjacent environment (e.g., substrate or electrolyte), and (iii) between graphene layers and their extended environment, which is separated from the layer by a certain number of additional graphene layers.

cond-mat.mtrl-sci↗

arXiv2018

Stress and charge transfer in uniaxially strained CVD graphene

Mechanical properties of graphene prepared by chemical vapor deposition (CVD) are not easily comparable to the properties of nearly perfect graphene prepared by mechanical cleavage. In this work, we attempt to investigate the mechanical performance of CVD graphene (simply supported or embedded in polymer matrix), transferred by two different techniques, under uniaxial loading with simultaneous in-situ monitoring by Raman microspectroscopy. The level of charge transfer doping and strain is assessed using the vector analysis modified for uniaxial strain. The strain distribution across the samples varies significantly, owing to the growth and transfer process, which induces wrinkles and faults in the CVD graphene. In simply supported specimens, the stress transfer efficiency is generally very low and the changes in Raman spectra are dominated by variations in the charge transfer originating from the realignment of the domains on the substrate upon the application of strain. In contrast, samples covered with an additional polymer layer exhibit an improved stress transfer efficiency, and the alterations of charge doping levels are negligible. In fully embedded specimens, the variations in stress transfer efficiencies are caused by the size of the effective graphene domains defined by cracks, folds and or/wrinkles.

cond-mat.mtrl-sci↗

arXiv2017

Wrinkled few-layer graphene as highly efficient load bearer

Multilayered graphitic materials are not suitable as load-bearers due to their inherent weak interlayer bonding (for example, graphite is a solid lubricant in certain applications). This situation is largely improved when two-dimensional (2-D) materials such as a monolayer (SLG) graphene are employed. The downside in these cases is the presence of thermally or mechanically induced wrinkles which are ubiquitous in 2-D materials. Here we set out to examine the effect of extensive large wavelength/ amplitude wrinkling on the stress transfer capabilities of exfoliated simply-supported graphene flakes. Contrary to common belief we present clear evidence that this type of "corrugation" enhances the load bearing capacity of few-layer graphene as compared to 'flat' specimens. This effect is the result of the significant increase of the graphene/polymer interfacial shear stress per increment of applied strain due to wrinkling and paves the way for designing affordable graphene composites with highly improved stress-transfer efficiency.

cond-mat.mtrl-sci↗