arXiv subjects

Ermin Malic

Publications and source records attributed to Ermin Malic.

At least 127 records · Page 7Linked to original sources

arXiv2017

Phonon Sidebands in Transition Metal Dichalcogenides

Excitons dominate the optical properties of monolayer transition metal dichalcogenides (TMDs). Besides optically accessible bright exciton states, TMDs exhibit also a multitude of optically forbidden dark excitons. Here, we show that efficient exciton-phonon scattering couples bright and dark states and gives rise to an asymmetric excitonic line shape. The observed asymmetry can be traced back to phonon-induced sidebands that are accompanied by a polaron redshift. We present a joint theory-experiment study investigating the microscopic origin of these sidebands in different TMD materials taking into account intra- and intervalley scattering channels opened by optical and acoustic phonons. The gained insights contribute to a better understanding of the optical fingerprint of these technologically promising nanomaterials.

cond-mat.mes-hall↗

arXiv2017

The role of momentum-dark excitons in the elementary optical response of bilayer WSe$_{2}$

Monolayer (ML) transition metal dichalcogenides (TMDs) undergo substantial changes in the single-particle band structure and excitonic optical response upon the addition of just one layer. As opposed to the single-layer limit, the bandgap of bilayer (BL) TMD semiconductors is indirect which results in reduced photoluminescence with richly structured spectra that have eluded a detailed understanding to date. Here, we provide a closed interpretation of the elementary optical responses of BL WSe$_2$ as a representative material for the wider class of TMD semiconductors. By combining theoretical calculations with comprehensive spectroscopy experiments, we identify the crucial role of momentum-indirect excitons for the understanding of basic absorption and emission spectra ubiquitously exhibited by various TMD BLs. Our results shed light on the origin of quantum dot (QD) formation in monolayer and bilayer crystals and will facilitate further advances directed at opto-electronic applications of layered TMD semiconductors in van der Waals heterostructures and devices.

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arXiv2017

Dark excitons in transition metal dichalcogenides

Monolayer transition metal dichalcogenides (TMDs) exhibit a remarkably strong Coulomb interaction that manifests in tightly bound excitons. Due to the complex electronic band structure exhibiting several spin-split valleys in the conduction and valence band, dark excitonic states can be formed. They are inaccessibly by light due to the required spin-flip and/or momentum transfer. The relative position of these dark states with respect to the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials and thus on their technological potential. Based on the solution of the Wannier equation, we present the excitonic landscape of the most studied TMD materials including the spectral position of momentum- and spin-forbidden excitonic states. We show that the knowledge of the electronic dispersion does not allow to conclude about the nature of the material's band gap, since excitonic effects can give rise to significant changes. Furthermore, we reveal that an exponentially reduced photoluminescence yield does not necessarily reflect a transition from a direct to a non-direct gap material, but can be ascribed in most cases to a change of the relative spectral distance between bright and dark excitonic states.

cond-mat.mtrl-sci↗

arXiv2017

Mapping of the dark exciton landscape in transition metal dichalcogenides

Transition metal dichalcogenides (TMDs) exhibit a remarkable exciton physics including optically accessible (bright) as well as spin- and momentum-forbidden (dark) excitonic states. So far the dark exciton landscape has not been revealed leaving in particular the spectral position of momentum-forbidden dark states completely unclear. This has a significant impact on the technological application potential of TMDs, since the nature of the energetically lowest state determines, if the material is a direct-gap semiconductor. Here, we show how dark states can be experimentally revealed by probing the intra-excitonic 1s-2p transition. Distinguishing the optical response shortly after the excitation (< 100$\,$fs) and after the exciton thermalization (> 1$\,$ps) allows us to demonstrate the relative position of bright and dark excitons. We find both in theory and experiment a clear blue-shift in the optical response demonstrating for the first time the transition of bright exciton populations into lower lying momentum- and spin-forbidden dark excitonic states in monolayer WSe$_2$.

cond-mat.mtrl-sci↗

arXiv2017

Impact of strain on the optical fingerprint of monolayer transition metal dichalcogenides

Strain presents a straightforward tool to tune electronic properties of atomically thin nanomaterials that are highly sensitive to lattice deformations. While the influence of strain on the electronic band structure has been intensively studied, there are only few works on its impact on optical properties of monolayer transition metal dichalcogenides (TMDs). Combining microscopic theory based on Wannier and Bloch equations with nearestneighbor tight-binding approximation, we present an analytical view on how uni- and biaxial strain influences the optical fingerprint of TMDs including their excitonic binding energy, oscillator strength, optical selection rules, and the radiative broadening of excitonic resonances. We show that the impact of strain can be reduced to changes in the lattice structure (geometric effect) and in the orbital functions (overlap effect). In particular, we demonstrate that the valley-selective optical selection rule is softened in the case of uniaxial strain due to the introduced asymmetry in the lattice structure. Furthermore, we reveal a considerable increase of the radiative dephasing due to strain-induced changes in the optical matrix element and the excitonic wave functions.

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arXiv2017

Current enhancement due to field-induced dark carrier multiplication in graphene

We present a microscopic study on current generation in graphene in response to an electric field. While scattering is generally considered to reduce the current, we reveal that in graphene Auger processes give rise to a current enhancement via a phenomenon we denote dark carrier multiplication. Based on a microscopic approach, we show that, if other scattering channels are absent, this prevents the carrier distribution to reach a stationary value. Taking into account scattering with phonons a finite current is restored, however its value exceeds the stationary current without scattering.

cond-mat.mes-hall↗

arXiv2017

Dark and bright exciton formation, thermalization, and photoluminescence in monolayer transition metal dichalcogenides

The remarkably strong Coulomb interaction in atomically thin transition metal dichalcogenides (TMDs) results in an extraordinarily rich many-particle physics including the formation of tightly bound excitons. Besides optically accessible bright excitonic states, these materials also exhibit a variety of dark excitons. Since they can even lie below the bright states, they have a strong influence on the exciton dynamics, lifetimes, and photoluminescence. While very recently, the presence of dark excitonic states has been experimentally demonstrated, the origin of these states, their formation, and dynamics have not been revealed yet. Here, we present a microscopic study shedding light on time- and energy-resolved formation and thermalization of bright and dark intra- and intervalley excitons as well as their impact on the photoluminescence in different TMD materials. We demonstrate that intervalley dark excitons, so far widely overlooked in current literature, play a crucial role in tungsten-based TMDs giving rise to an enhanced photoluminescence and reduced exciton lifetimes at elevated temperatures.

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arXiv2016

Out of the dark and into the light: towards dark-state based chemical sensors

The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light-matter interaction results in a high sensitivity to changes in their surrounding. Here, we present a novel, highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical finger print for the detection of molecules - in contrast to common sensing schemes relying on small peak shifts and intensity changes.

cond-mat.mtrl-sci↗

arXiv2016

Review on carrier multiplication in graphene

The remarkable gapless and linear band structure of graphene opens up new carrier relaxation channels bridging the valence and the conduction band. These Auger scattering processes change the number of charge carriers and can give rise to a significant multiplication of optically excited carriers in graphene. This is an ultrafast many-particle phenomenon that is of great interest both for fundamental many-particle physics as well as technological applications. Here, we review the research on carrier multiplication in graphene and Landau-quantized graphene including theoretical modelling and experimental demonstration.

cond-mat.mes-hall↗

arXiv2016

Unconventional double-bended saturation of optical transmission in graphene due to many-particle interactions

We present a joint theory-experiment study on the transmission/absorption saturation after ultrafast pulse excitation in graphene. We reveal an unconventional double-bended saturation behavior: Both bendings separately follow the standard saturation model exhibiting two saturation fluences, however, the corresponding fluences differ by three orders of magnitude and have different physical origin. Our results reveal that this new and unexpected behavior can be ascribed to an interplay between fluence- and time-dependent many-particle scattering processes and phase-space filling effects.

cond-mat.mes-hall↗

arXiv2016

Proposal for a tunable graphene-based terahertz Landau-level laser

In the presence of strong magnetic fields the electronic bandstructure of graphene drastically changes. The Dirac cone collapses into discrete non-equidistant Landau levels, which can be externally tuned by changing the magnetic field. In contrast to conventional materials, specific Landau levels are selectively addressable using circularly polarized light. Exploiting these unique properties, we propose the design of a tunable laser operating in the technologically promising terahertz spectral range. To uncover the many-particle physics behind the emission of light, we perform a fully quantum mechanical investigation of the non-equilibrium dynamics of electrons, phonons, and photons in optically pumped Landau-quantized graphene embedded into an optical cavity. The gained microscopic insights allow us to predict optimal experimental conditions to realize a technologically promising terahertz laser.

cond-mat.mes-hall↗

arXiv2016

Optical fingerprint of dark 2p-states in transition metal dichalcogenides

We present a microscopic study on higher excitonic states in transition metal dichalcogenides in the presence of disorder. We show that the geometric phase cancels the degeneration of 2s and 2p states and that a significant disorder-induced coupling of bright and dark states offers a strategy to circumvent optical selection rules. As a prove, we show a direct fingerprint of dark 2p states in absorption spectra of WS$_2$. The predicted softening of optical selection rules through exciton-disorder coupling is of general nature and therefore applicable to related two-dimensional semiconductors.

cond-mat.mtrl-sci↗

arXiv2016

Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS$_2$ and MoSe$_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS$_2$ through phonon emission at all temperatures.

cond-mat.mtrl-sci↗

arXiv2015

Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides

We report charged exciton (trion) formation dynamics in doped monolayer transition metal dichalcogenides (TMDs), specifically molybdenum diselenide (MoSe2), using resonant two-color pump-probe spectroscopy. When resonantly pumping the exciton transition, trions are generated on a picosecond timescale through exciton-electron interaction. As the pump energy is tuned from the high energy to low energy side of the inhomogeneously broadened exciton resonance, the trion formation time increases by ~ 50%. This feature can be explained by the existence of both localized and delocalized excitons in a disordered potential and suggests the existence of an exciton mobility edge in TMDs. The quasiparticle formation and conversion processes are important for interpreting photoluminescence and photoconductivity in TMDs.

cond-mat.mes-hall↗

arXiv2015

Impact of doping on the carrier dynamics in graphene

We present a microscopic study on the impact of doping on the carrier dynamics in graphene, in particular focusing on its influence on the technologically relevant carrier multiplication in realistic, doped graphene samples. Treating the time- and momentum-resolved carrier-light, carrier-carrier, and carrier-phonon interactions on the same microscopic footing, the appearance of Auger-induced carrier multiplication up to a Fermi level of 300 meV is revealed. Furthermore, we show that doping favors the so-called hot carrier multiplication occurring within one band. Our results are directly compared to recent time-resolved ARPES measurements and exhibit an excellent agreement on the temporal evolution of the hot carrier multiplication for n- and p-doped graphene. The gained insights shed light on the ultrafast carrier dynamics in realistic, doped graphene samples

cond-mat.mes-hall↗

arXiv2014

Microscopic view on the ultrafast photoluminescence from photo-excited graphene

We present a joint theory-experiment study on ultrafast photoluminescence from photoexcited graphene. Based on a microscopic theory, we reveal two distinct mechanisms behind the occurring photoluminescence: Besides the well-known incoherent contribution driven by non-equilibrium carrier occupations, we found a coherent part that spectrally shifts with the excitation energy. In our experiments, we demonstrate for the first time the predicted appearance and spectral shift of the coherent photoluminescence.

cond-mat.mes-hall↗

arXiv2014

Carrier multiplication in graphene under Landau quantization

Carrier multiplication is a many-particle process giving rise to the generation of multiple electron-hole pairs. This process holds the potential to increase the power conversion efficiency of photovoltaic devices. In graphene, carrier multiplication has been theoretically predicted and recently experimentally observed. However, due to the absence of a bandgap and competing phonon-induced electron-hole recombination, the extraction of charge carriers remains a substantial challenge. Here we present a new strategy to benefit from the gained charge carriers by introducing a Landau quantization that offers a tunable bandgap. Based on microscopic calculations within the framework of the density matrix formalism, we report a significant carrier multiplication in graphene under Landau quantization. Our calculations reveal a high tunability of the effect via externally accessible pump fluence, temperature, and the strength of the magnetic field.

cond-mat.mes-hall↗

arXiv2014

Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides

Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions. Using optical coherent two-dimensional spectroscopy, we provide the first experimental determination of the exciton homogeneous linewidth in monolayer transition metal dichalcogenides, specifically tungsten diselenide (WSe2). The role of exciton-exciton and exciton-phonon interactions in quantum decoherence is revealed through excitation density and temperature dependent linewidth measurements. The residual homogeneous linewidth extrapolated to zero density and temperature is ~1.5 meV, placing a lower bound of approximately 0.2 ps on the exciton radiative lifetime. The exciton quantum decoherence mechanisms presented in this work are expected to be ubiquitous in atomically-thin semiconductors.

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