| 1. |
- Berghäuser, Gunnar, 1983, et al.
(författare)
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Inverted valley polarization in optically excited transition metal dichalcogenides
- 2018
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 9:1
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Tidskriftsartikel (refereegranskat)abstract
- Large spin-orbit coupling in combination with circular dichroism allows access to spin-polarized and valley-polarized states in a controlled way in transition metal dichalcogenides. The promising application in spin-valleytronics devices requires a thorough understanding of intervalley coupling mechanisms, which determine the lifetime of spin and valley polarizations. Here we present a joint theory-experiment study shedding light on the Dexter-like intervalley coupling. We reveal that this mechanism couples A and B excitonic states in different valleys, giving rise to an efficient intervalley transfer of coherent exciton populations. We demonstrate that the valley polarization vanishes and is even inverted for A excitons, when the B exciton is resonantly excited and vice versa. Our theoretical findings are supported by energy-resolved and valley-resolved pump-probe experiments and also provide an explanation for the recently measured up-conversion in photoluminescence. The gained insights might help to develop strategies to overcome the intrinsic limit for spin and valley polarizations.
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| 2. |
- Berghäuser, Gunnar, 1983, et al.
(författare)
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Mapping of the dark exciton landscape in transition metal dichalcogenides
- 2018
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Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 98:2
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Tidskriftsartikel (refereegranskat)abstract
- Transition metal dichalcogenides (TMDs) exhibit a remarkable exciton physics including bright and optically forbidden dark excitonic states. Here, we show how dark excitons can be experimentally revealed by probing the intraexcitonic 1s-2p transition. Distinguishing the optical response shortly after the excitation and after the exciton thermalization allows us to reveal the relative position of bright and dark excitons. We find both in theory and experiment a clear blueshift in the optical response demonstrating the transition of bright exciton populations into lower-lying dark excitonic states.
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| 3. |
- Berghäuser, Gunnar, 1983, et al.
(författare)
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Optical fingerprint of dark 2p-states in transition metal dichalcogenides
- 2017
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Ingår i: 2D Materials. - : IOP Publishing. - 2053-1583. ; 4:1
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Tidskriftsartikel (refereegranskat)abstract
- Atomically thin transition metal dichalcogenides exhibit a remarkably strong Coulomb interaction. This results in a fascinating many-particle physics including a variety of bright and dark excitonic states that determine optical and electronic properties of these materials. So far, the impact of dark states has remained literally in the dark to a large extent, since a measurement of these optically forbidden states is very challenging. Here we demonstrate a strategy to measure a direct fingerprint of dark states even in standard linear absorption spectroscopy. We present a microscopic study on bright and dark higher excitonic states in the presence of disorder for the exemplary material of tungsten disulfide (WS2). We show that the geometric phase cancels the degeneration of 2s and 2p states and that a significant disorder-induced coupling of these bright and dark states offers a strategy to circumvent optical selection rules. As a proof, we show a clear fingerprint of dark 2p states in the absorption spectrum of WS2. The predicted softening of optical selection rules through exciton-disorder coupling is of general nature and therefore applicable to related two-dimensional semiconductors.
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| 4. |
- Bernal, Ivan, 1984, et al.
(författare)
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Exciton broadening and band renormalization due to Dexter-like intervalley coupling
- 2018
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Ingår i: 2D Materials. - : IOP Publishing. - 2053-1583. ; 5:2
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Tidskriftsartikel (refereegranskat)abstract
- A remarkable property of atomically thin transition metal dichalcogenides (TMDs) is the possibility to selectively address single valleys by circularly polarized light. In the context of technological applications, it is very important to understand possible intervalley coupling mechanisms. Here, we show how the Dexter-like intervalley coupling mixes A and B states from opposite valleys leading to a significant broadening γB 1s of the B 1s exciton. The effect is much more pronounced in tungsten-based TMDs, where the coupling excitonic states are quasi-resonant. We calculate a ratio γB B 1s /γA B 1s ≈ 4.0, which is in good agreement with the experimentally measured value of 3.9 ± 0.7. In addition to the broadening effect, the Dexter-like intervalley coupling also leads to a considerable energy renormalization resulting in an increased energetic distance between A 1s and B 1s states.
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| 5. |
- Brem, Samuel, 1991, et al.
(författare)
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Exciton Relaxation Cascade in two-dimensional Transition Metal Dichalcogenides
- 2018
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322 .- 2045-2322. ; 8:1
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Tidskriftsartikel (refereegranskat)abstract
- Monolayers of transition metal dichalcogenides (TMDs) are characterized by an extraordinarily strong Coulomb interaction giving rise to tightly bound excitons with binding energies of hundreds of meV. Excitons dominate the optical response as well as the ultrafast dynamics in TMDs. As a result, a microscopic understanding of exciton dynamics is the key for a technological application of these materials. In spite of this immense importance, elementary processes guiding the formation and relaxation of excitons after optical excitation of an electron-hole plasma has remained unexplored to a large extent. Here, we provide a fully quantum mechanical description of momentum- and energy-resolved exciton dynamics in monolayer molybdenum diselenide (MoSe2) including optical excitation, formation of excitons, radiative recombination as well as phonon-induced cascade-like relaxation down to the excitonic ground state. Based on the gained insights, we reveal experimentally measurable features in pump-probe spectra providing evidence for the exciton relaxation cascade.
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| 6. |
- Christiansen, D., et al.
(författare)
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Phonon Sidebands in Monolayer Transition Metal Dichalcogenides
- 2017
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Ingår i: Physical Review Letters. - 1079-7114 .- 0031-9007. ; 119:18
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Tidskriftsartikel (refereegranskat)abstract
- 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.
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| 7. |
- Feierabend, Maja, 1990, et al.
(författare)
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Dark exciton based strain sensing in tungsten-based transition metal dichalcogenides
- 2019
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Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 99:19
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Tidskriftsartikel (refereegranskat)abstract
- The recent emergence of atomically thin two-dimensional (2D) materials has opened up possibilities for the design of ultrathin and flexible nanoelectronic devices. As truly 2D materials, they exhibit an optimal surface-to-volume ratio, which results in an extremely high sensitivity to external changes which can not be achieved by conventional semiconductors. This makes these materials optimal candidates for sensing applications. Here, we propose a dark exciton based concept for ultrasensitive strain sensors. By investigating both dark and bright excitons in tungsten-based monolayer transition metal dichalcogenides, we demonstrate that the dark-bright-exciton separation can be controlled by strain, which has a crucial impact on the activation of dark excitonic states. The predicted opposite strain-induced shifts for dark and bright excitons result in a pronounced change in photoluminescence stemming from dark excitons even at very small strain values. The predicted high optical gauge factors of up to 8000 are promising for the design of optical strain sensors.
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| 8. |
- Feierabend, Maja, 1990, et al.
(författare)
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Impact of strain on the optical fingerprint of monolayer transition-metal dichalcogenides
- 2017
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Ingår i: Physical Review B. - 2469-9969 .- 2469-9950. ; 96:4
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Tidskriftsartikel (refereegranskat)abstract
- 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 a few works on its impact on optical properties of monolayer transition-metal dichalcogenides (TMDs). Combining microscopic theory based on Wannier and Bloch equations with nearest-neighbor 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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| 9. |
- Feierabend, Maja, 1990, et al.
(författare)
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Molecule signatures in photoluminescence spectra of transition metal dichalcogenides
- 2018
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Ingår i: Physical Review Materials. - 2475-9953. ; 2:1
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Tidskriftsartikel (refereegranskat)abstract
- Monolayer transition metal dichalcogenides (TMDs) show an optimal surface-to-volume ratio and are thus promising candidates for novel molecule sensor devices. It was recently predicted that a certain class of molecules exhibiting a large dipole moment can be detected through the activation of optically inaccessible (dark) excitonic states in absorption spectra of tungsten-based TMDs. In this paper, we investigate the molecule signatures in photoluminescence spectra in dependence of a number of different experimentally accessible quantities, such as excitation density, temperature, as well as molecular characteristics including the dipole moment and its orientation, molecule-TMD distance, molecular coverage, and distribution. We show that under certain optimal conditions even room-temperature detection of molecules can be achieved.
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| 10. |
- Feierabend, Maja, 1990, et al.
(författare)
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Optical fingerprint of non-covalently functionalized transition metal dichalcogenides
- 2017
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Ingår i: Journal of Physics Condensed Matter. - 0953-8984 .- 1361-648X. ; 29:38, s. Article no 384003 -
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Tidskriftsartikel (refereegranskat)abstract
- Atomically thin transition metal dichalcogenides (TMDs) hold promising potential forapplications in optoelectronics. Due to their direct band gap and the extraordinarily strong Coulomb interaction, TMDs exhibit efficient light-matter coupling and tightly bound excitons. Moreover, large spin orbit coupling in combination with circular dichroism allows for spin and valley selective optical excitation. As atomically thin materials, they are very sensitive to changes in the surrounding environment. This motivates a functionalization approach, where external molecules are adsorbed to the materials surface to tailor its optical properties. Here, we apply the density matrix theory to investigate the potential of non-covalently functionalized monolayer TMDs. Considering exemplary molecules with a strong dipole moment, we predict spectral redshifts and the appearance of an additional side peak in the absorption spectrum of functionalized TMDs. We show that the molecular characteristics, e.g. coverage, orientation and dipole moment, crucially influence the optical properties of TMDs, leaving a unique optical fingerprint in the absorption spectrum. Furthermore, we find that the molecular dipole moments open a channel for coherent intervalley coupling between the high-symmetry K and K' points which may create new possibilities for spin-valleytronics application.
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