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Register a new userNon-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
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Monolayers (MLs) of MoS2 and WSe2 are 2D semiconductors with strong, direct optical transitions that are governed by tightly Coulomb bound eletron-hole pairs (excitons). The optoelectronic properties of these transition metal dichalcogenides are directly related to the inherent crystal inversion symmetry breaking. It allows for efficient second harmonic generation (SHG) and is at the origin of chiral optical selections rules, which enable efficient optical initialization of electrons in specific K-valleys in momentum space. Here we demonstrate how these unique non-linear and linear optical properties can be combined to efficiently prepare exciton valley coherence and polarization through resonant pumping of an excited exciton state. In particular a new approach to coherent alignment of excitons following two-photon excitation is demonstrated. We observe a clear deviation of the excited exciton spectrum from the standard Rydberg series via resonances in SHG spectroscopy and two- and one-photon absorption. The clear identification of the 2s and 2p exciton excited states combined with first principle calculations including strong anti-screening effects allows us to determine an exciton binding energy of the order of 600 meV in ML WSe2.
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The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A-exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing to extrapolate an exciton binding energy of about 220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.
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 direct gap interband transitions in transition metal dichalcogenides monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the $K^+$ or $K^-$ valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30 degrees in applied fields up to 9 T. This exciton valley coherence control on ps time scale could be an important step towards complete control of qubits based on the valley degree of freedom.
We experimentally demonstrate hot exciton transport in h-BN encapsulated WSe2 monolayers via spatially and temporally resolved photoluminescence measurements at room temperature. We show that the nonlinear evolution of the mean squared displacement of the non-resonantly excited hot exciton gas is primarily due to the relaxation of its excess kinetic energy and is characterized by a density-dependent fast expansion that converges to a slower, constant rate expansion. We also observe saturation of the hot exciton gas expansion rate at high excitation densities due to the balance between Auger-assisted hot exciton generation and the phonon-assisted hot exciton relaxation processes.
Nonlinear optical phenomena are widely used for the study of semiconductor materials. The paper presents an overview of experimental and theoretical studies of excitons by the method of optical second and third harmonics generation in various bulk semiconductors (GaAs, CdTe, ZnSe, ZnO, Cu$_2$O, (Cd,Mn)Te, EuTe, EuSe), and low-dimensional heterostructures ZnSe/BeTe. Particular attention is paid to the role of external electric and magnetic fields that modify the exciton states and induce new mechanisms of optical harmonics generation. Microscopic mechanisms of harmonics generation based on the Stark effect, the spin and orbital Zeeman effects, and on the magneto-Stark effect specific for excitons moving in an external magnetic field are considered. This approach makes it possible to study the properties of excitons and to obtain new information on their energy and spin structure that is not available when the excitons are investigated by linear optical spectroscopy. As a result of these studies, a large amount of information was obtained, which allows us to conclude on the establishing of a new field of research - exciton spectroscopy by the method of optical harmonics generation.
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