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Ermin Malic Dissertation

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You are free to opt out any time or opt in for other cookies to get a better experience. A clear experimental evidence for the existence of darkexcitonic states below the A1s exciton in TMD materials canbe obtained by measuring the temperature dependence of the 014002-4 Page 6. Note that one finds for every spin-like statean energetically degenerated spin-unlike state in the correspondingopposite valley. The same as in Fig. 1, however, now considering.

ACKNOWLEDGMENTS We acknowledge financial support from the Swedish Re-search Council, the Stiftelsen Olle Engkvist, the DeutscheForschungsgemeinschaft (DFG) through SFB 787 and SFB910, and the Chalmers Area of Advance in Nanoscienceand Nanotechnology. The researchers have applied for a patent for the new sensor mechanism, and are now working to demonstrate the proposal experimentally. The coefficientscan be obtained by solving the Schrodinger equation forthe free-particle Hamiltonian including the spin-orbit inter-action. An increase of therelative spectral distance between bright and dark excitonicstates of approximately 100 meV already results in a decreaseof the PL yield by two orders of magnitude. If the loweststate is bright, then the quantum yield will be maximal at 0 Kand will then decrease at higher temperature. In addition to momentumforbidden dark states, there isalso a different class of dark excitons based on the spin. Note that the dashed linescorrespond to the relative band ordering in the free-particle picture. We show that the experimentallyobserved increase in the quantum yield for monolayer TMDsdoes not necessarily reflect a transition from indirect to directgap semiconductors, but can be explained by a change inthe relative spectral position of bright and dark states. The calculation of theseparameters is beyond the scope of this work. According to Fig. 3, we estimate therelative increase of dark-bright splitting from mono to bilayerMoS2 to be 140 meV. Adding a twist angle one can externally tune these moire potentials, which presents a unique opportunity to design tailored. The coefficientscan be obtained by solving the Schrodinger equation forthe free-particle Hamiltonian including the spin-orbit interaction. A clear experimental evidence for the existence of darkexcitonic states below the A1s exciton in TMD materials canbe obtained by measuring the temperature dependence of the 014002-4 Page 6. These coefficients in- clude the lattice-dependent symmetries and the resulting elec-tronic band structure at the high symmetry points in theBrillouin zone of the investigated TMD material. The initiative, which builds on the previous 10-years of the Graphene Flagship, is funded by the European Commission’s Horizon Europe research and innovation programme. The precise characteristics of the peak should depend on factors such as molecular coverage, polarity of the gas molecule, and distance between the molecule and the sensor. Due to the complex electronic band structure exhibiting several spin-splitvalleys in the conduction and valence band, dark excitonic states can be formed. Therefore, the spin-orbit-coupling-induced differencesstem only from the conduction band. For TMDs, it is of crucial importance toaccount for excitonic effects. As a result, at very low temperatures,we find the typical behavior for an indirect semiconductor,i.e., an increase in the quantum yield with temperature, cf.the dashed purple line in Fig. 4(a). However, above a certaintemperature around 100 K, we find a turning point and thequantum yield decreases again reflecting the behavior of adirect-gap semiconductor. Please be aware that this might heavily reduce the functionality and appearance of our site. We show that the knowledge of the electronic dispersion does not allow to conclude about thenature of the material’s band gap since excitonic effects can give rise to significant changes. The calculation of theseparameters is beyond the scope of this work. If you refuse cookies we will remove all set cookies in our domain. The increasing quantum yield of MoS2 can be ascribedto the energetically lowest ?-K exciton states, which arepredominantly occupied at low temperatures. Furthermore, wedistinguish K-hole and ?-hole states, where the hole is locatedeither at the K valley (Fig. 1) or at the ? valley (Fig. 2). Thecorresponding electron can then be either in the ?(?) or the K (?)valley.

The relative position of these dark states with respectto the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials andthus on their technological potential. Additionally, they alsoexhibit spin-forbidden excitonic states well below the brightA1s exciton, cf. Figs. 1(c) and 1(e). The spin-forbidden K-Kexciton, consisting of Coulomb-bound electrons and holesboth located in the K valley but with the opposite spin, lieapproximately 50 meV below the bright state for WS2 andWSe2 on a SiO2 substrate. Spin-up and spin-down bands are denoted by red and blue lines,respectively. Both effects cancelto a large extent and are small in a typical doping regimes of1011 cm?2. In the latter case, one can expect theimpact on the relative difference of excitonic states to berelatively small. The goal is to shed lighton the relative spectral position of bright as well as momentum-and spin-forbidden dark excitonic states and investigate theirimpact on the photoluminescence (PL) quantum yield. In addition to momentum-forbidden dark states, there isalso a different class of dark excitons based on the spin. Similarly to the hydrogen problem, we introduce center-of-mass and relative momenta Q and q, respectively. The impactof doping on excitonic properties in this case only dependson the phase-space filling, which induces a renormalizationof the band gap and the Rabi frequency. You always can block or delete cookies by changing your browser settings and force blocking all cookies on this website. The center-of-mass momentum Q isdetermined by the difference of the momenta k1,k2 of the twobound particles. We show that the experimentallyobserved increase in the quantum yield for monolayer TMDsdoes not necessarily reflect a transition from indirect to directgap semiconductors, but can be explained by a change inthe relative spectral position of bright and dark states. These coefficients in- clude the lattice-dependent symmetries and the resulting elec-tronic band structure at the high symmetry points in theBrillouin zone of the investigated TMD material. Quantumyield for monolayer (a) MoS2, WS2 and (b) MoSe2, WSe2 as afunction of temperature. Dashedlines reflect the relative band ordering in a free-particle picturewithout taking into account excitonic binding energies. The relative position of these dark states with respectto the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials andthus on their technological potential. While inmolybdenum-based TMDs, the bright exciton is the energeticallylowest state (yellow line), tungsten-based TMDs exhibit lower lyingdark excitonic states. Using fully quantum mechanical models, we microscopically. Schematic electronic dispersions around the K and. In particular, environmental sensing of different types of gases is highly relevant for security and safety applications, including detecting pollution. As a result, at very low temperatures,we find the typical behavior for an indirect semiconductor,i.e., an increase in the quantum yield with temperature, cf.the dashed purple line in Fig. 4(a). However, above a certaintemperature around 100 K, we find a turning point and thequantum yield decreases again reflecting the behavior of adirect-gap semiconductor. In the last step, we assume that the bright state lies well abovethe dark states, i.e., ? db ? ??1. In this situation, we findan exponential decrease of the PL quantum yield with therelative dark-bright separation ? db. As a result, thetemperature dependence is a clear indication for the nature ofthe band gap. For TMDs, it is of crucial importance toaccount for excitonic effects. The electronic bandstructure of TMDs exhibits four distinguished minima in theenergetically lowest conduction band (K, K ?, ?, and ??)and three maxima in the highest valence band (K, K ?, and?). Wewould like to emphasize that the focus of our work doesnot lie on exact quantitative numbers for a specific TMD,but on revealing qualitative trends induced by the excitonlandscape and their implications on experimentally accessibleparameters, such as the photoluminescence quantum yield.

III.

EXCITON

LANDSCAPE Evaluating the Wannier equation, we have full access tothe eigenenergies of all exciton states. The relative position of dark and brightexcitonic states in a TMD material can be directly read off bythe temperature dependence of the quantum yield. Dashedlines reflect the relative band ordering in a free-particle picturewithout taking into account excitonic binding energies. Interestingly, we findin tungsten-based TMDs dark excitons energetically belowthe bright K-K transition (orange dashed lines), i.e., these 014002-3 Page 5. The strong Coulomb interaction gives rise to spatially separated.

The initiative, which builds on the previous 10-years of the Graphene Flagship, is funded by the European Commission’s Horizon Europe research and innovation programme. The relative motionis determined by the total momentum of the bound electronsand holes. Here, we define Q with respect to the holemomentum, i.e., it gives the relative position of the electron inmomentum space with respect to the hole. In the first case, thelowest conduction and the highest valence band have the oppositespin. According to Fig. 3, we estimate therelative increase of dark-bright splitting from mono to bilayerMoS2 to be 140 meV. The impactof doping on excitonic properties in this case only dependson the phase-space filling, which induces a renormalizationof the band gap and the Rabi frequency. The precise characteristics of the peak should depend on factors such as molecular coverage, polarity of the gas molecule, and distance between the molecule and the sensor. In the Wannier equation,we introduced the attractive electron-hole contribution of theCoulomb interactionV cq,vkck,vq and the electron (hole) occupations fe?(h?)q. You can check these in your browser security settings. The strong optical response of TMDs is particularly promising for sensing using light. In addition to momentum-forbidden dark states, there isalso a different class of dark excitons based on the spin. The calculation of theseparameters is beyond the scope of this work.

Figures 1 (c) to 1(f)show the excitonic dispersion including the lowest A1s excitonstates in the four most studied TMD materials (MoS2, MoSe2,WS2, and WSe2). ACKNOWLEDGMENTS We acknowledge financial support from the Swedish Re-search Council, the Stiftelsen Olle Engkvist, the DeutscheForschungsgemeinschaft (DFG) through SFB 787 and SFB910, and the Chalmers Area of Advance in Nanoscienceand Nanotechnology. The quantum yield is extremelysensitive to db and shows an exponential dependence (except forthe region around db ? 0) reflecting the Boltzmann distribution ofexcitonic states. Q NA1s Q ?Q,kpt, where kpt isthe photon momentum, determined by the speed of lightc and the photon frequency kpt. Please be aware that this might heavily reduce the functionality and appearance of our site. The effective masses resulting from thelattice symmetry and spacial orbital overlaps are in all TMDsthe smallest at the K point followed by the. The coefficientscan be obtained by solving the Schrodinger equation forthe free-particle Hamiltonian including the spin-orbit inter-action. Finally, we discuss the temperature dependence of thequantum yield. Interestingly, we findin tungsten-based TMDs dark excitons energetically belowthe bright KK transition (orange dashed lines), i.e., these 014002-3 Page 5. Since the splitting dueto the shortrange intra- and intervalley electron-hole exchangeinteraction does not influence the relative position of darkand bright states, it is not important for the present studyfocusing on the effect of dark and bright exciton positionson experimentally accessible parameters. Additionally, they alsoexhibit spinforbidden excitonic states well below the brightA1s exciton, cf. Figs. 1(c) and 1(e). The spinforbidden K-Kexciton, consisting of Coulomb-bound electrons and holesboth located in the K valley but with the opposite spin, lieapproximately 50 meV below the bright state for WS2 andWSe2 on a SiO2 substrate. Thus, we only find spin- and momentum-forbidden dark excitonstates. The search for novel structures with new functionalities has brought atomically. Thislast is dominated by bright excitons well below the quasifreeparticle band gap. The increasing quantum yield of MoS2 can be ascribedto the energetically lowest ?-K exciton states, which arepredominantly occupied at low temperatures. Quantumyield for monolayer (a) MoS2, WS2 and (b) MoSe2, WSe2 as afunction of temperature. If you refuse cookies we will remove all set cookies in our domain. We include all momentum-and spin-forbidden dark excitonic states.

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