arXiv subjects

Ermin Malic

Publications and source records attributed to Ermin Malic.

At least 73 records · Page 4Linked to original sources

arXiv2022

Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe$_2$ bilayers

While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ valley to other lower energy $Γ$ and $Λ$ valleys in the bilayer. Our combined experimental and theoretical studies unequivocally establish different microscopic mechanisms that determine exciton quantum dynamics in TMDC monolayers and bilayers. Understanding exciton quantum dynamics provides critical guidance to manipulation of spin/valley degrees of freedom in TMDC bilayers.

cond-mat.mes-hall↗

arXiv2022

Singlet exciton optics and phonon-mediated dynamics in oligoacene semiconductor crystals

Organic semiconductor crystals stand out as an efficient, cheap and diverse platform for realising optoelectronic applications. The optical response of these crystals is governed by a rich tapestry of exciton physics. So far, little is known on the phonon-driven singlet exciton dynamics in this class of materials. In this joint theory-experiment work, we combine the fabrication of a high-quality oligoacene semiconductor crystal and characterization via photoluminescence measurements with a sophisticated approach to the microscopic modeling in these crystals. This allows us to investigate singlet exciton optics and dynamics. We predict phonon-bottleneck effects in pentacene crystals, where we find dark excitons acting as crucial phonon-mediated relaxation scattering channels. While the efficient singlet fission in pentacene crystals hampers the experimental observation of this bottleneck effect, we reveal both in theory and experiment a distinct polarisation- and temperature-dependence in absorption and photoluminescence spectra of tetracene crystals, including microscopic origin of exciton linewidths, the activation of the higher Davydov states at large temperatures, and polarisation-dependent quenching of specific exciton resonances. Our joint theory-experiment study represents a significant advance in microscopic understanding of singlet exciton optics and dynamics in oligoacene crystals.

cond-mat.mes-hall↗

arXiv2022

Exciton transport in a moiré potential: from hopping to dispersive regime

The propagation of excitons in TMD monolayers has been intensively studied revealing interesting many-particle effects, such as halo formation and non-classical diffusion. Initial studies have investigated how exciton transport changes in twisted TMD bilayers, including Coulomb repulsion and Hubbard-like exciton hopping. In this work, we investigate the twist-angle-dependent transition of the hopping regime to the dispersive regime of effectively free excitons. Based on a microscopic approach for excitons in the presence of a moiré potential, we show that the hopping regime occurs up to an angle of approximately 2° and is well described by the Hubbard model. At large angles, however, the Hubbard model fails due to increasingly delocalized exciton states. Here, the quantum mechanical dispersion of free particles with an effective mass determines the propagation of excitons. Overall, our work provides microscopic insights into the character of exciton propagation in twisted van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2022

Ultrafast phonon-driven charge transfer in van der Waals heterostructures

Van der Waals heterostructures built by vertically stacked transition metal dichalcogenides (TMDs) exhibit a rich energy landscape including interlayer and intervalley excitons. Recent experiments demonstrated an ultrafast charge transfer in TMD heterostructures. However, the nature of the charge transfer process has remained elusive. Based on a microscopic and material-realistic exciton theory, we reveal that phonon-mediated scattering via strongly hybridized intervalley excitons governs the charge transfer process that occurs on a sub-100fs timescale. We track the time-, momentum-, and energy-resolved relaxation dynamics of optically excited excitons and determine the temperature- and stacking-dependent charge transfer time for different TMD bilayers. The provided insights present a major step in microscopic understanding of the technologically important charge transfer process in van der Waals heterostructures.

cond-mat.mes-hall↗

arXiv2022

Trion-phonon interaction in atomically thin semiconductors

Optical and transport properties of doped monolayer semiconductors are dominated by trions, which are three-particle compounds formed by two electrons and one hole or vice versa. In this work, we investigate the trion-phonon interaction on a microscopic footing and apply our model to the exemplary case of a molybdenum diselenide (MoSe2) monolayer. We determine the trion series of states and their internal quantum structure by solving the trion Schrödinger equation. Transforming the system into a trion basis and solving equations of motion, including the trion-phonon interaction within the second-order Born-Markov approximation, provides a microscopic access to the trion dynamics. In particular, we investigate trion propagation and compute the diffusion coefficient and mobility. In the low density limit, we find that trions propagate less efficiently than excitons and electrons due to their stronger coupling with phonons and their larger mass. For increasing densities, we predict a drastic enhancement of diffusion caused by the build-up of a large pressure by the degenerate trion gas, which is a direct consequence of the fermionic character of trions. Our work provides microscopic insights into the trion-phonon interaction and its impact on the diffusion behaviour in atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2022

Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides

Integrating 2D materials into high-quality optical microcavities opens the door to fascinating many-particle phenomena including the formation of exciton-polaritons. These are hybrid quasi-particles inheriting properties of both the constituent photons and excitons. In this work, we investigate the so-far overlooked impact of dark excitons on the momentum-resolved absorption spectra of hBN-encapsulated WSe$_2$ and MoSe$_2$ monolayers in the strong-coupling regime. In particular, thanks to the efficient phonon-mediated scattering of polaritons into energetically lower dark exciton states, the absorption of the lower polariton branch in WSe$_2$ is much higher than in MoSe$_2$. It shows unique step-like increases in the momentum-resolved profile indicating opening of specific scattering channels. We study how different externally accessible quantities, such as temperature or mirror reflectance, change the optical response of polaritons. Our study contributes to an improved microscopic understanding of exciton-polaritons and their interaction with phonons, potentially suggesting experiments that could determine the energy of dark exciton states via momentum-resolved polariton absorption.

cond-mat.mes-hall↗

arXiv2022

Flat-band-induced many-body interactions and exciton complexes in a layered semiconductor

Interactions among a collection of particles generate many-body effects in solids resulting in striking modifications of material properties. The heavy carrier mass that yields strong interactions and gate control of carrier density over a wide range, make two-dimensional semiconductors an exciting playground to explore many-body physics. The family of III-VI metal monochalcogenides emerges as a new platform for this purpose due to its excellent optical properties and the flat valence band dispersion with a Mexican-hat-like inversion. In this work, we present a complete study of charge-tunable excitons in few-layer InSe by photoluminescence spectroscopy. From the optical spectra, we establish that free excitons in InSe are more likely to be captured by ionized donors due to the large exciton Bohr radius, leading to the formation of bound exciton complexes. Surprisingly, a pronounced redshift of the exciton energy accompanied by a decrease of the exciton binding energy upon hole-doping reveals a significant band gap renormalization and dynamical screening induced by the presence of the Fermi reservoir. Our findings establish InSe as a reproducible and potentially manufacturable platform to explore electron correlation phenomena without the need for twist-angle engineering.

cond-mat.mes-hall↗

arXiv2022

Microscopic origin of anomalous interlayer exciton transport in van der Waals heterostructures

Van der Waals heterostructures constitute a platform for investigating intriguing many-body quantum phenomena. In particular, transition-metal dichalcogenide (TMD) hetero-bilayers host long-lived interlayer excitons which exhibit permanent out-of-plane dipole moments. Here, we develop a microscopic theory for interlayer exciton-exciton interactions including both the dipolar nature of interlayer excitons as well as their fermionic substructure, which gives rise to an attractive fermionic exchange. We find that these interactions contribute to a drift force resulting in highly non-linear exciton propagation at elevated densities in the MoSe$_2$-WSe$_2$ heterostructure. We show that the propagation can be tuned by changing the number of hBN spacers between the TMD layers or by adjusting the dielectric environment. In particular, although counter-intuitive, we reveal that interlayer excitons in free-standing samples propagate slower than excitons in hBN-encapsulated TMDs - due to an enhancement of the net Coulomb-drift with stronger environmental screening. Overall, our work contributes to a better microscopic understanding of the interlayer exciton transport in technologically promising atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2022

Electrical tuning of moiré excitons in MoSe$_2$ bilayers

Recent advances in the field of vertically stacked 2D materials have revealed a rich exciton landscape. In particular, it has been demonstrated that out-of-plane electrical fields can be used to tune the spectral position of spatially separated interlayer excitons. Other studies have shown that there is a strong hybridization of exciton states, resulting from the mixing of electronic states in both layers. However, the connection between the twist-angle dependent hybridization and field-induced energy shifts has remained in the dark. Here, we investigate on a microscopic footing the interplay of electrical and twist-angle tuning of moiré excitons in MoSe$_2$ homobilayers. We reveal distinct energy regions in PL spectra that are clearly dominated by either intralayer or interlayer excitons, or even dark excitons. Consequently, we predict twist-angle-dependent critical electrical fields at which the material is being transformed from a direct into an indirect semiconductor. Our work provides new microscopic insights into experimentally accessible knobs to significantly tune the moiré exciton physics in atomically thin nanomaterials.

cond-mat.mes-hall↗

arXiv2022

Interlayer exciton landscape in WS$_2$/tetracene heterostructures

The vertical stacking of two-dimensional materials into heterostructures gives rise to a plethora of intriguing optoelectronic properties and presents an unprecedented potential for technological development. While much progress has been made combining different monolayers of transition metal dichalgonenides (TMDs), little is known about TMD-based heterostructures including organic layers of molecules. Here, we present a joint theory-experiment study on a TMD/tetracene heterostructure demonstrating clear signatures of spatially separated interlayer excitons in low temperature photoluminescence spectra. Here, the Coulomb-bound electrons and holes are localized either in the TMD or in the molecule layer, respectively. In particular, we reveal both in theory and experiment signatures of the entire intra- and interlayer exciton landscape in the photoluminescence spectra. In particular, we find both in theory and experiment a pronounced transfer of intensity from the intralayer TMD exciton to a series of energetically lower interlayer excitons with decreasing temperature. In addition, we find signatures phonon-sidebands stemming from these interlayer exciton states. Our findings shed light on the microscopic nature of interlayer excitons in TMD/molecule heterostructures and could have important implications for technological applications of these materials.

cond-mat.mes-hall↗

arXiv2022

The moiré potential in twisted transition metal dichalcogenide bilayers

Moiré superlattices serve as a playground for emerging phenomena, such as localization of band states, superconductivity, and localization of excitons. These superlattices are large and are often modeled in the zero angle limit, which obscures the effect of finite twist angles. Here, by means of first-principles calculations we quantify the twist-angle dependence of the moiré potential in the MoS$_2$ homobilayer and identify the contributions from the constituent elements of the moiré potential. Furthermore, by considering the zero-angle limit configurations, we show that the moiré potential is rather homogeneous across the transition metal dichalcogenides (TMDs) and briefly discuss the separate effects of potential shifts and hybridization on the bilayer hybrid excitons. We find that the moiré potential in TMDs exhibits both an electrostatic component and a hybridization component, which are intertwined and have different relative strengths in different parts of the Brillouin zone. The electrostatic component of the moiré potential is a varying dipole field, which has a strong twist angle dependence. In some cases, the hybridization component can be interpreted as a tunneling rate but the interpretation is not generally applicable over the full Brillouin zone.

cond-mat.mtrl-sci↗

arXiv2022

Microscopic modelling of exciton-polariton diffusion coefficients in atomically thin semiconductors

In the strong light-matter coupling regime realized e.g. by integrating semiconductors into optical microcavities, polaritons as new hybrid light-matter quasi-particles are formed. The corresponding change in the dispersion relation has a large impact on optics, dynamics and transport behaviour of semiconductors. In this work, we investigate the strong-coupling regime in hBN-encapsulated MoSe$_2$ monolayers focusing on exciton-polariton diffusion. Applying a microscopic approach based on the exciton density matrix formalism combined with the Hopfield approach, we predict a drastic increase of the diffusion coefficients by two to three orders of magnitude in the strong coupling regime. We explain this behaviour by the much larger polariton group velocity and suppressed polariton-phonon scattering channels with respect to the case of bare excitons. Our study contributes to a better microscopic understanding of polariton diffusion in atomically thin semiconductors.

cond-mat.mtrl-sci↗

arXiv2022

Twist Angle Tuning of Moiré Exciton Polaritons in van der Waals Heterostructures

Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been in the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist angle. We find that these new hybrid light-exciton states become delocalized relative to the constituent excitons due to the mixing with light and higher-energy excitons. The system can be interpreted as a natural quantum metamaterial with a periodicity that can be engineered via the twist angle. Our study presents a significant advance in microscopic understanding and control of moiré exciton polaritons in twisted atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2022

Exciton landscape in van der Waals heterostructures

van der Waals heterostructures consisting of vertically stacked transition-metal dichalcogenides (TMDs) exhibit a rich landscape of bright and dark intra- and interlayer excitons. In spite of a growing literature in this field of research, the type of excitons dominating optical spectra in different van der Waals heterostructures has not yet been well established. The spectral position of exciton states depends strongly on the strength of hybridization and energy renormalization due to the periodic moiré potential. Combining exciton density-matrix formalism and density-functional theory, we shed light on the exciton landscape in TMD homo- and heterobilayers at different stackings. This allows us to identify on a microscopic footing the energetically lowest-lying exciton state for each material and stacking. Furthermore, we disentangle the contribution of hybridization and layer polarization-induced alignment shifts of dark and bright excitons in photoluminescence spectra. By revealing the exciton landscape in van der Waals heterostructures, our work provides the basis for further studies of the optical, dynamical, and transport properties of this technologically promising class of nanomaterials.

cond-mat.mes-hall↗

arXiv2021

Dark exciton-exciton annihilation in monolayer WSe$_2$

The exceptionally strong Coulomb interaction in semiconducting transition-metal dichalcogenides (TMDs) gives rise to a rich exciton landscape consisting of bright and dark exciton states. At elevated densities, excitons can interact through exciton-exciton annihilation (EEA), an Auger-like recombination process limiting the efficiency of optoelectronic applications. Although EEA is a well-known and particularly important process in atomically thin semiconductors determining exciton lifetimes and affecting transport at elevated densities, its microscopic origin has remained elusive. In this joint theory-experiment study combining microscopic and material-specific theory with time- and temperature-resolved photoluminescence measurements, we demonstrate the key role of dark intervalley states that are found to dominate the EEA rate in monolayer WSe$_2$. We reveal an intriguing, characteristic temperature dependence of Auger scattering in this class of materials with an excellent agreement between theory and experiment. Our study provides microscopic insights into the efficiency of technologically relevant Auger scattering channels within the remarkable exciton landscape of atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2021

Terahertz fingerprint of monolayer Wigner crystals

The strong Coulomb interaction in monolayer semiconductors represents a unique opportunity for the realization of Wigner crystals without external magnetic fields. In this work, we predict that the formation of monolayer Wigner crystals can be detected by their terahertz response spectrum, which exhibits a characteristic sequence of internal optical transitions. We apply the density matrix formalism to derive the internal quantum structure and the optical conductivity of the Wigner crystal and to microscopically analyze the multi-peak shape of the obtained terahertz spectrum. Moreover, we predict a characteristic shift of the peak position as function of charge density for different atomically thin materials and show how our results can be generalized to an arbitrary two-dimensional system.

cond-mat.str-el↗

arXiv2021

Valley-exchange coupling probed by angle-resolved photoluminescence

The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field due to the valley-specific Zeeman-shift. We propose that angle-dependent photoluminescence measurements involving both circular and linear optical polarisation as well as magnetic fields should act as strong verification of the role of valley-exchange coupling on excitonic dispersionand its signatures in optical spectra

cond-mat.mes-hall↗

arXiv2021

Nonclassical Exciton Diffusion in Monolayer WSe2

We experimentally demonstrate time-resolved exciton propagation in a monolayer semiconductor at cryogenic temperatures. Monitoring phonon-assisted recombination of dark states, we find a highly unusual case of exciton diffusion. While at 5 K the diffusivity is intrinsically limited by acoustic phonon scattering, we observe a pronounced decrease of the diffusion coefficient with increasing temperature, far below the activation threshold of higher-energy phonon modes. This behavior corresponds neither to well-known regimes of semiclassical free-particle transport nor to the thermally activated hopping in systems with strong localization. Its origin is discussed in the framework of both microscopic numerical and semi-phenomenological analytical models illustrating the observed characteristics of nonclassical propagation. Challenging the established description of mobile excitons in monolayer semiconductors, these results open up avenues to study quantum transport phenomena for excitonic quasiparticles in atomically-thin van der Waals materials and their heterostructures.

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