No Arabic abstract
Interfacing atomically thin van der Waals semiconductors with magnetic substrates enables additional control on their intrinsic valley degree of freedom and provides a promising platform for the development of novel valleytronic devices for information processing and storage. Here we study circularly polarized photoluminescence in heterostructures of monolayer MoSe$_2$ and thin films of ferrimagnetic bismuth iron garnet. We observe strong emission from charged excitons with negative valley polarization, which switches sign with increasing temperature, and demonstrate contrasting response to left and right circularly polarized excitation, associated with finite out-of-plane magnetization in the substrate. We propose a theoretical model accounting for magnetization-induced imbalance of charge carriers in the two valleys of MoSe$_2$, as well as for valley-switching scattering from B to A excitons and fast formation of trions with extended valley relaxation times, which shows excellent agreement with the experimental data. Our results provide new insights into valley physics in 2D semiconductors interfaced with magnetic substrates.
We study the impact of a free carrier reservoir on the optical properties of excitonic and trionic complexes in a MoSe$_2$ monolayer at cryogenic temperatures. By applying photodoping via a non-resonant pump laser the electron density can be controlled in our sample and in turn the exciton and trion densities can be tuned. We find a significant increase of the trion binding energy in the presence of an induced electron gas both in power- and in time-resolved photoluminescence spectra. This behaviour is reproduced within the original variational approach that takes into account both screening and phase space filling effects.
Monolayer transition metal dichalcogenides (TMDs) hold great promise for future information processing applications utilizing a combination of electron spin and valley pseudospin. This unique spin system has led to observation of the valley Zeeman effect in neutral and charged excitonic resonances under applied magnetic fields. However, reported values of the trion valley Zeeman splitting remain highly inconsistent across studies. Here, we utilize high quality hBN encapsulated monolayer WSe$_2$ to enable simultaneous measurement of both intervalley and intravalley trion photoluminescence. We find the valley Zeeman splitting of each trion state to be describable only by a combination of three distinct g-factors, one arising from the exciton-like valley Zeeman effect, the other two, trion specific, g-factors associated with recoil of the excess electron. This complex picture goes significantly beyond the valley Zeeman effect reported for neutral excitons, and eliminates the ambiguity surrounding the magneto-optical response of trions in tungsten based TMD monolayers.
The valley pseudospin in monolayer transition metal dichalcogenides (TMDs) has been proposed as a new way to manipulate information in various optoelectronic devices. This relies on a large valley polarization that remains stable over long timescales (hundreds of ns). However, time resolved measurements report valley lifetimes of only a few ps. This has been attributed to mechanisms such as phonon-mediated inter-valley scattering and a precession of the valley psedospin through electron-hole exchange. Here we use transient spin grating to directly measure the valley depolarization lifetime in monolayer MoSe$_{2}$. We find a fast valley decay rate that scales linearly with the excitation density at different temperatures. This establishes the presence of strong exciton-exciton Coulomb exchange interactions enhancing the valley depolarization. Our work highlights the microscopic processes inhibiting the efficient use of the exciton valley pseudospin in monolayer TMDs.
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.
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.