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تسجيل مستخدم جديدDiffusivity Reveals Three Distinct Phases of Interlayer Excitons in MoSe2/WSe2 Heterobilayers
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Charge separated interlayer excitons in transition metal dichalcogenide (TMDC) heterobilayers are being explored for moire exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the MoSe2/WSe2 heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moire-potential to the modestly mobile exciton gas as exciton density increases to ne/h ~ 1011 cm-2 and from the exciton gas to the highly mobile charge separated electron/hole plasma for ne/h > 1012 cm-2. The latter is the Mott transition and is confirmed in photoconductivity measurements. These findings set fundamental limits for achieving quantum states of interlayer excitons.
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Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can
be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, with bound electrons and holes localized in individual monolayers, i.e. interlayer excitons. Here, we report the first observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by both photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity of interlayer excitons are highly tunable by an applied vertical gate voltage, implying electrical control of the heterojunction band-alignment. Using time resolved photoluminescence, we find that the interlayer exciton is long-lived with a lifetime of about 1.8 ns, an order of magnitude longer than intralayer excitons13-16. Our work demonstrates the ability to optically pump interlayer electric polarization and provokes the immediate exploration of interlayer excitons for condensation phenomena, as well as new applications in 2D light-emitting diodes, lasers, and photovoltaic devices.
MoSe2-WSe2 heterostructures host strongly bound interlayer excitons (IXs) which exhibit bright photoluminescence (PL) when the twist-angle is near 0{deg} or 60{deg}. Over the past several years, there have been numerous reports on the optical respons
e of these heterostructures but no unifying model to understand the dynamics of IXs and their temperature dependence. Here, we perform a comprehensive study of the temperature, excitation power, and time-dependent PL of IXs. We observe a significant decrease in PL intensity above a transition temperature that we attribute to a transition from localized to delocalized IXs. Astoundingly, we find a simple inverse relationship between the IX PL energy and the transition temperature, which exhibits opposite power dependent behaviors for near 0{deg} and 60{deg} samples. We conclude that this temperature dependence is a result of IX-IX exchange interactions, whose effect is suppressed by the moire potential trapping IXs at low temperature.
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly
hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and triplet interlayer excitons show giant valley-Zeeman splitting between the K and K valleys, a result of the large Lande g-factor of the singlet interlayer exciton and triplet interlayer exciton, which are experimentally determined to be ~ 10.7 and ~ 15.2, respectively, in good agreement with theoretical expectation. The PL from the singlet and triplet interlayer excitons show opposite helicities, determined by the atomic registry. Helicity-resolved photoluminescence excitation (PLE) spectroscopy study shows that both singlet and triplet interlayer excitons are highly valley-polarized at the resonant excitation, with the valley polarization of the singlet interlayer exciton approaches unity at ~ 20 K. The highly valley-polarized singlet and triplet interlayer excitons with giant valley-Zeeman splitting inspire future applications in spintronics and valleytronics.
Stripe phases, in which the rotational symmetry of charge density is spontaneously broken, occur in many strongly correlated systems with competing interactions. One representative example is the copper-oxide superconductors, where stripe order is th
ought to be relevant to the mechanism of high-temperature superconductivity. Identifying and studying the stripe phases in conventional strongly correlated systems are, however, challenging due to the complexity and limited tunability of these materials. Here we uncover stripe phases in WSe2/WS2 moire superlattices with continuously gate-tunable charge densities by combining optical anisotropy and electronic compressibility measurements. We find strong electronic anisotropy over a large doping range peaked at 1/2 filling of the moire superlattice. The 1/2-state is incompressible and assigned to a (insulating) stripe crystal phase. It can be continuously melted by thermal fluctuations around 35 K. The domain configuration revealed by wide-field imaging shows a preferential alignment along the high-symmetry axes of the moire superlattice. Away from 1/2 filling, we observe additional stripe crystals at commensurate filling 1/4, 2/5 and 3/5. The anisotropy also extends into the compressible regime of the system at incommensurate fillings, indicating the presence of electronic liquid crystal states. The observed filling-dependent stripe phases agree with the theoretical phase diagram of the extended Hubbard model on a triangular lattice in the flat band limit. Our results demonstrate that two-dimensional semiconductor moire superlattices are a highly tunable platform to study the stripe phases and their interplay with other symmetry breaking ground states.
We investigate the optical properties of spin-triplet interlayer excitons in heterobilayer transition metal dichalcogenides in comparison with the spin-singlet ones. Surprisingly, the optical transition dipole of the spin-triplet exciton is found to
be in the same order of magnitude to that of the spin-singlet exciton, in sharp contrast to the monolayer excitons where the spin triplet species is considered as dark compared to the singlet. Unlike the monolayer excitons whose spin-conserved (spin-flip) transition dipole can only couple to light of in-plane (out-of-plane) polarization, such restriction is removed for the interlayer excitons due to the breaking of the out-of-plane mirror symmetry. We find that as the interlayer atomic registry changes, the optical transition dipole of interlayer exciton crosses between in-plane ones of opposite circular polarization and the out-of-plane one for both the spin-triplet and spin-singlet species. As a result, excitons of both species have non-negligible coupling into photon modes of both in-plane and out-of-plane propagations, another sharp difference from the monolayers where the exciton couples predominantly into the out-of-plane propagation channel. At given atomic registry, the spin-triplet and spin-singlet excitons have distinct valley polarization selection rules, allowing the selective optical addressing of both the valley configuration and the spin singlet/triplet configuration of interlayer excitons.
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