9 research outputs found
Phonon-assisted exciton and trion conversion efficiency in transition metal Dichalcogenides
Photoluminescence spectra, shows that monolayer Transition-metal
dichalcogenides (MLTMDCs), possess charged exciton binding energies,
conspicuously similar to the energy of optical phonons. This enigmatic
coincidence has offered opportunities to investigate many-body interactions
between trion, exciton and phonon and led to efficient excitonic anti-Stokes
processes with the potential for laser refrigeration and energy harvesting. In
this study, we show that in WSe2 materials, the trion binding energy matches
two phonon modes, the outofplane HP and the in-plane LO mode. In this respect,
using the Fermi golden rule together with the effective mass approximation, we
investigate the rate of the population transfers between exciton and trion,
mediated by a single phonon. We demonstrate that, while the absolute importance
of the two phonon modes on the upconversion process strongly depend on the
experimental conditions such as the temperature and the dielectric environment
(substrate), both modes lead to an up-conversion process on time scales in the
range of few picoseconds to sub-nanosecond, consistent with recents
experimental findings. The conjugate process is also investigated in our study,
as a function of temperature and electron density . We prove that exciton to
trion down-conversion process is very unlikely at low electron density and high
temperature while it increases dramatically to reach few picoseconds time scale
at low temperature and for electron density . Finally, our results show that
conversion process occurs more rapidly in exemplary monolayer molybdenum-based
dichalcogenides (MoSe2 and MoTe2) than tungsten dichalcogenides .Comment: 29 page,6figures,articl
Radiative lifetime of localized excitons in transition metal dichalcogenides
Disorder derived from defects or strain in monolayer TMDs can lead to a
dramatic change in the physical behavior of the interband excitations,
producing inhomogeneous spectral broadening and localization; leading to
radiative lifetime increase. In this study, we have modeled the disorder in the
surface of the sample through a randomized potential in monolayer WSe2. We show
that this model allows us to simulate the spectra of localized exciton states
as well as their radiative lifetime. In this context, we give an in depth study
of the influence of the disorder potential parameters on the optical properties
of these defects through energies, density of states, oscillator strengths,
photoluminescence (PL) spectroscopy and radiative lifetime at low temperature
(4K). We demonstrate that localized excitons have a longer emission time than
free excitons, in the range of tens of picoseconds or more, and we show that it
depends strongly on the disorder parameter and dielectric environment. Finally,
in order to prove the validity of our model we compare it to available
experimental results of the literature.Comment: arXiv admin note: text overlap with arXiv:1409.3996 by other author
Tuning trion binding energy and oscillator strength in a laterally finite 2D system: CdSe nanoplatelets as a model system for trion properties
We present a theoretical study combined with experimental validations demonstrating that CdSe nanoplatelets are a model system to investigate the tunability of trions and excitons in laterally finite 2D semiconductors. Our results show that the trion binding energy can be tuned from 36 meV to 18 meV with the lateral size and decreasing aspect ratio, while the oscillator strength ratio of trions to excitons decreases. In contrast to conventional quantum dots, the trion oscillator strength in a nanoplatelet at low temperature is smaller than that of the exciton. The trion and exciton Bohr radii become lateral size tunable, e.g. from âŒ3.5 to 4.8 nm for the trion. We show that dielectric screening has strong impact on these properties. By theoretical modeling of transition energies, binding energies and oscillator strength of trions and excitons and comparison with experimental findings, we demonstrate that these properties are lateral size and aspect ratio tunable and can be engineered by dielectric confinement, allowing to suppress e.g. detrimental trion emission in devices. Our results strongly impact further in-depth studies, as the demonstrated lateral size tunable trion and exciton manifold is expected to influence properties like gain mechanisms, lasing, quantum efficiency and transport even at room temperature due to the high and tunable trion binding energies.EC/H2020/714876/EU/Photonics in Flatland: Band Structure Engineering of 2D Excitons in Fluorescent Colloidal Nanomaterials/PHOCONATU Berlin, Open-Access-Mittel - 202
The optical absorption in indirect semiconductor to semimetal PtSe2 arises from direct transitions
is a van der Waals material transiting from an indirect
semiconductor to a semimetal with increasing thickness. Its absorption
threshold has been conjectured to originate from interband indirect
transitions. By quantitative comparison between wideband optical absorption
() of high-quality exfoliated crystals and ab-initio
simulations, we prove instead that the optical absorption arises only from
direct transitions. This understanding allows us to shed new light on the
semiconductor to semimetal transition and to explore the effect of stacking and
excitons on optical absorption
Atomic Layer-controlled Nonlinear Terahertz Valleytronics in Dirac Semi-metal and Semiconductor PtSe2
Platinum diselenide (PtSe2) is a promising two-dimensional (2D) material for
the terahertz (THz) range as, unlike other transition metal dichalcogenides
(TMDs), its bandgap can be uniquely tuned from a semiconductor in the
near-infrared to a semimetal with the number of atomic layers. This gives the
material unique THz photonic properties that can be layer-engineered. Here, we
demonstrate that a controlled THz nonlinearity - tuned from monolayer to bulk
PtSe2 - can be realised in wafer size polycrystalline PtSe2 through the
generation of ultrafast photocurrents and the engineering of the bandstructure
valleys. This is combined with the PtSe2 layer interaction with the substrate
for a broken material centro-symmetry permitting a second order nonlinearity.
Further, we show layer-dependent circular dichroism, where the sign of the
ultrafast currents and hence the phase of the emitted THz pulse can be
controlled through the excitation of different bandstructure valleys. In
particular, we show that a semimetal has a strong dichroism that is absent in
the monolayer and few layer semiconducting limit. The microscopic origins of
this TMD bandstructure engineering is highlighted through detailed DFT
simulations and show that circular dichroism can be controlled when PtSe2
becomes a semimetal and when the K-valleys can be excited. As well as showing
that PtSe2 is a promising material for THz generation through layer controlled
optical nonlinearities, this work opens up new class of circular dichroism
materials beyond the monolayer limit that has been the case of traditional
TMDs, and impacting a range of domains from THz valleytronics, THz spintronics
to harmonic generation
Radiative lifetime of localized excitons in transition-metal dichalcogenides
International audienceDisorder derived from defects or local strain in monolayer transition-metal dichalcogenides (TMDs) can lead to a dramatic change in the physical behavior of the interband excitations, producing inhomogeneous spectral broadening and localization leading to radiative lifetime increase. In this study, we have modeled the surface disorder of a monolayer TMD sample through a randomized potential in the layer plane. We show that this model, applied to a monolayer of WSe2, allows us to simulate the spectra of localized exciton states as well as their radiative lifetime. In this context, we give an in depth study of the influence of the disorder potential parameters on the optical properties of these defects through energies, density of states, oscillator strengths, photoluminescence (PL) spectroscopy, and radiative lifetime at low temperature (4 K). We demonstrate that localized excitons have a longer emission time than free excitons, in the range of tens of picoseconds or more, the radiative decay time depending strongly on the disorder parameter and dielectric environment. Finally, in order to prove the validity of our model, we compare it to available experimental results of the literature
Radiative lifetime of localized excitons in transition-metal dichalcogenides
International audienceDisorder derived from defects or local strain in monolayer transition-metal dichalcogenides (TMDs) can lead to a dramatic change in the physical behavior of the interband excitations, producing inhomogeneous spectral broadening and localization leading to radiative lifetime increase. In this study, we have modeled the surface disorder of a monolayer TMD sample through a randomized potential in the layer plane. We show that this model, applied to a monolayer of WSe2, allows us to simulate the spectra of localized exciton states as well as their radiative lifetime. In this context, we give an in depth study of the influence of the disorder potential parameters on the optical properties of these defects through energies, density of states, oscillator strengths, photoluminescence (PL) spectroscopy, and radiative lifetime at low temperature (4 K). We demonstrate that localized excitons have a longer emission time than free excitons, in the range of tens of picoseconds or more, the radiative decay time depending strongly on the disorder parameter and dielectric environment. Finally, in order to prove the validity of our model, we compare it to available experimental results of the literature
Tuning exciton diffusion, mobility and emission line width in CdSe nanoplatelets via lateral size
We investigate the lateral size tunability of the exciton diffusion coefficient and mobility in colloidal quantum wells by means of line width analysis and theoretical modeling. We show that the exciton diffusion coefficient and mobility in laterally finite 2D systems like CdSe nanoplatelets can be tuned via the lateral size and aspect ratio. The coupling to acoustic and optical phonons can be altered via the lateral size and aspect ratio of the platelets. Subsequently the exciton diffusion and mobility become tunable since these phonon scattering processes determine and limit the mobility. At 4 K the exciton mobility increases from ⌠4 Ă 103 cm2 Vâ1 sâ1 to more than 1.4 Ă 104 cm2 Vâ1 sâ1 for large platelets, while there are weaker changes with size and the mobility is around 8 Ă 101 cm2 Vâ1 sâ1 for large platelets at room temperature. In turn at 4 K the exciton diffusion coefficient increases with the lateral size from ⌠1.3 cm2 sâ1 to ⌠5 cm2 sâ1, while it is around half the value for large platelets at room temperature. Our experimental results are in good agreement with theoretical modeling, showing a lateral size and aspect ratio dependence. The findings open up the possibility for materials with tunable exciton mobility, diffusion or emission line width, but quasi constant transition energy. High exciton mobility is desirable e.g. for solar cells and allows efficient excitation harvesting and extraction.TU Berlin, Open-Access-Mittel â 202
Layer-controlled nonlinear terahertz valleytronics in two-dimensional semimetal and semiconductor PtSeâ
Platinum diselenide ((Formula presented.)) is a promising two-dimensional (2D) material for the terahertz (THz) range as, unlike other transition metal dichalcogenides (TMDs), its bandgap can be uniquely tuned from a semiconductor in the near-infrared to a semimetal with the number of atomic layers. This gives the material unique THz photonic properties that can be layer-engineered. Here, we demonstrate that a controlled THz nonlinearityâtuned from monolayer to bulk (Formula presented.) âcan be realized in wafer size polycrystalline (Formula presented.) through the generation of ultrafast photocurrents and the engineering of the bandstructure valleys. This is combined with the (Formula presented.) layer interaction with the substrate for a broken material centrosymmetry, permitting a second order nonlinearity. Further, we show layer dependent circular dichroism, where the sign of the ultrafast currents and hence the phase of the emitted THz pulse can be controlled through the excitation of different bandstructure valleys. In particular, we show that a semimetal has a strong dichroism that is absent in the monolayer and few layer semiconducting limit. The microscopic origins of this TMD bandstructure engineering are highlighted through detailed DFT simulations, and shows the circular dichroism can be controlled when (Formula presented.) becomes a semimetal and when the K-valleys can be excited. As well as showing that (Formula presented.) is a promising material for THz generation through layer controlled optical nonlinearities, this work opens up a new class of circular dichroism materials beyond the monolayer limit that has been the case of traditional TMDs, and impacting a range of domains from THz valleytronics, THz spintronics to harmonic generation.National Research Foundation (NRF)Published versionThis work was funded by H2020 Future and Emerging Technologies, Grant/Award Number:964735; H2020 Excellent Science, Grant/Award Number: 881603; Agence Nationale de la Recherche, Grant/Award Numbers: ANR-16-CE24-0023, ANR-2018-CE08-018-05; National Research Foundation Singapore, Grant/Award Number: NRF-CRP26-2021-0004; Region Ile de France; Equip Meso, Grant/Award Number: ANR-10-EQPX-29-01