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Register a new userLandau-quantized excitonic absorption and luminescence in a monolayer valley semiconductor
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We investigate Landau-quantized excitonic absorption and luminescence of monolayer WSe$_2$ under magnetic field. We observe gate-dependent quantum oscillations in the bright exciton and trions (or exciton-polarons) as well as the dark trions and their phonon replicas. Our results reveal spin- and valley-polarized Landau levels (LLs) with filling factors $n = +0, +1$ in the bottom conduction band and $n = -0$ to $-6$ in the top valence band, including the Berry-curvature-induced $n = pm0$ LLs of massive Dirac fermions. The LL filling produces periodic plateaus in the exciton energy shift accompanied by sharp oscillations in the exciton absorption width and magnitude. This peculiar exciton behavior can be simulated by semi-empirical calculations. The experimentally deduced g-factors of the conduction band (g ~ 2.5) and valence band (g ~ 15) exceed those predicted in a single-particle model (g = 1.5, 5.5, respectively). Such g-factor enhancement implies strong many-body interactions in gated monolayer WSe$_2$. The complex interplay between Landau quantization, excitonic effects, and many-body interactions makes monolayer WSe$_2$ a promising platform to explore novel correlated quantum phenomena.
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The coupling between spin, charge, and lattice degrees of freedom plays an important role in a wide range of fundamental phenomena. Monolayer semiconducting transitional metal dichalcogenides have emerged as an outstanding platform for studying these coupling effects because they possess unique spin-valley locking physics for hosting rich excitonic species and the reduced screening for strong Coulomb interactions. Here, we report the observation of multiple valley phonons, phonons with momentum vectors pointing to the corners of the hexagonal Brillouin zone, and the resulting exciton complexes in the monolayer semiconductor WSe2. From Lande g-factor and polarization analyses of photoluminescence peaks, we find that these valley phonons lead to efficient intervalley scattering of quasi particles in both exciton formation and relaxation. This leads to a series of photoluminescence peaks as valley phonon replicas of dark trions. Using identified valley phonons, we also uncovered an intervalley exciton near charge neutrality, and extract its short-range electron-hole exchange interaction to be about 10 meV. Our work not only identifies a number of previously unknown 2D excitonic species, but also shows that monolayer WSe2 is a prime candidate for studying interactions between spin, pseudospin, and zone-edge phonons.
Due to degeneracies arising from crystal symmetries, it is possible for electron states at band edges (valleys) to have additional spin-like quantum numbers. An important question is whether coherent manipulation can be performed on such valley pseudospins, analogous to that routinely implemented using true spin, in the quest for quantum technologies. Here we show for the first time that SU(2) valley coherence can indeed be generated and detected. Using monolayer semiconductor WSe2 devices, we first establish the circularly polarized optical selection rules for addressing individual valley excitons and trions. We then reveal coherence between valley excitons through the observation of linearly polarized luminescence, whose orientation always coincides with that of any linearly polarized excitation. Since excitons in a single valley emit circularly polarized photons, linear polarization can only be generated through recombination of an exciton in a coherent superposition of the two valleys. In contrast, the corresponding photoluminescence from trions is not linearly polarized, consistent with the expectation that the emitted photon polarization is entangled with valley pseudospin. The ability to address coherence, in addition to valley polarization, adds a critical dimension to the quantum manipulation of valley index necessary for coherent valleytronics.
The newly discovered valley degree of freedom (DOF) in atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDs) offers a promising platform to explore rich nonlinear physics, such as spinor Bose-Einstein condensate (BEC) and novel valleytronics applications. However, the critical nonlinear effect, such as valley polariton bosonic stimulation (BS), has long remained an unresolved challenge due to the generation of limited polariton ground state densities necessary to induce the stimulated scattering of polaritons in specific valleys. Here, we report, for the first time, the valley bosonic stimulation of exciton-polaritons via spin-valley locking in a WS2 monolayer microcavity. This is achieved by the resonant injection of valley polaritons at specific energy and wavevector, which allows spin-polarized polaritons to efficiently populate their ground state and induce a valley-dependent bosonic stimulation. As a result, we observe the nonlinear self-amplification of polariton emission from the valley-dependent ground state. Our finding paves the way for both fundamental study of valley polariton BEC physics and non-linear optoelectronic devices such as spin-dependent parametric oscillators and spin-lasers.
We report magneto-absorption spectroscopy of gated WSe$_2$ monolayers in high magnetic fields up to 60~T. When doped with a 2D Fermi sea of mobile holes, well-resolved sequences of optical transitions are observed in both $sigma^pm$ circular polarizations, which unambiguously and separately indicate the number of filled Landau levels (LLs) in both $K$ and $K$ valleys. This reveals the interaction-enhanced valley Zeeman energy, which is found to be highly tunable with hole density $p$. We exploit this tunability to align the LLs in $K$ and $K$, and find that the 2D hole gas becomes unstable against small changes in LL filling and can spontaneously valley-polarize. These results cannot be understood within a single-particle picture, highlighting the importance of exchange interactions in determining the ground state of 2D carriers in monolayer semiconductors.
Non-equilibrium dynamics of strongly correlated systems constitutes a fascinating problem of condensed matter physics with many open questions. Here we investigate the relaxation dynamics of Landau-quantized electron system into spin-valley polarized ground state in a gate-tunable MoSe$_2$ monolayer subjected to a strong magnetic field. The system is driven out of equilibrium with optically injected excitons that depolarize the electron spins and the subsequent electron spin-valley relaxation is probed in time-resolved experiments. We demonstrate that the relaxation rate at millikelvin temperatures sensitively depends on the Landau level filling factor: it becomes faster whenever the electrons form an integer quantum Hall liquid and slows down appreciably at non-integer fillings. Our findings evidence that valley relaxation dynamics may be used as a tool to investigate the interplay between the effects of disorder and strong interactions in the electronic ground state.
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