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We present femtosecond pump-probe measurements of neutral and charged exciton optical response in monolayer MoSe2to resonant photoexcitation of a given exciton state in the presence of 2D electron gas. We show that creation of charged exciton (X−) population in a given K+, K−valley requires the capture of available free carriers in the opposite valley and reduces the interaction of neutral exciton (X) with the electron Fermi sea. We also observe spectral broadening of the X transition line with the increasing X−population caused by efficient scattering and excitation induced dephasing. From the valley-resolved analysis of the observed effects we are able to extract the spin-valley relaxation times of free carriers as a function of carrier density. Moreover, we analyze the oscillator strength and energy shift of X in the regime of interaction with electron Fermi sea under resonant excitation. From this we can observe the process of X decay by radiative recombination paired with trion formation. We demonstrate an increase of neutral exciton relaxation rate with the introduction of Fermi sea of electrons. We ascribe the observed effect to the increased efficiency of the trion formation, as well as the radiative decay caused by the screening of disorder by the free carriers.

Competition between exchange interactions and magnetocrystalline anisotropy may bring new magnetic states that are of great current interest. An applied hydrostatic pressure can further be used to tune their balance. In this work, we investigate the magnetization process of a biaxial antiferromagnet in an external magnetic field applied along the easy axis. We find that the single metamagnetic transition of the Ising type observed in this material under ambient pressure transforms under hydrostatic pressure into two transitions, a first-order spin-flop transition followed by a second-order transition toward a polarized ferromagnetic state near saturation. This reversible tuning into a new magnetic phase is obtained in layered bulk CrSBr at low temperature by varying the interlayer distance using high hydrostatic pressure, which efficiently acts on the interlayer magnetic exchange and is probed by magneto-optical spectroscopy.

We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS3. Our measurements reveal an excitation that closely resembles the antiferromagnetic resonance mode typical of easy-axis antiferromagnets; nevertheless, it displays an unusual, four-times larger Zeeman splitting in an applied magnetic field. We identify this excitation with an |Sz| = 4 multipolar magnon─a single-ion 4-magnon bound state─that corresponds to a full reversal of a single magnetic moment of the Fe2+ion. We argue that condensation of multipolar magnons in large-spin materials with a strong magnetic anisotropy can produce new exotic states.

Using ultrafast resonant pump-probe spectroscopy in an unconventional experimental setup we investigate the spectral shape and dynamics of absorption features related to the A exciton in an hexagonal boron nitride (hBN)/MoSe2/hBN van der Waals heterostructure. While in a pure two-level system a pump-probe experiment measures the occupation or the polarization dynamics, depending on the time ordering of the pulse pair, in the transition metal dichalcogenide (TMD) system both quantities get thoroughly mixed by strong exciton–exciton interaction. We find that for short positive delays the spectral lines experience pronounced changes in their shape and energy and they relax to the original situation on a picosecond time scale. For negative delays, distinctive spectral oscillations appear indicating the first-time observation of perturbed free induction decay for a TMD system. The comparison between co-circular and cross-circular excitation schemes further allows us to investigate the rapid inter-valley scattering. By considering a three-level system as a minimal model including the local field effect, excitation-induced dephasing (EID), and scattering between the excited states we explain all phenomena observed in the experiment with excellent consistency. Our handy model can be even further reduced to two levels in the case of a co-circular excitation, for which we derive analytic expressions to describe the detected signals. This allows us to trace back the spectral shapes and shifts to the impact of local field effect and EID thus fully reproducing the complex behavior of the observed effects.

We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of n-doped WS2monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically inactive complexes. The semidark trions and negative biexcitons are distinguished. On the basis of their experimentally extracted and theoretically calculated g-factors, we identify three distinct families of emissions due to exciton complexes in WS2: bright, intravalley, and intervalley dark. The g-factors of the spin-split subbands in both the conduction and valence bands are also determined.

Monolayer transition-metal dichalcogenides (TMDs) manifest exceptional optical properties related to narrow excitonic resonances. However, these properties have been so far explored only for structures produced by techniques inducing considerable large-scale inhomogeneity. In contrast, techniques which are essentially free from this disadvantage, such as molecular beam epitaxy (MBE), have to date yielded only structures characterized by considerable spectral broadening, which hinders most of the interesting optical effects. Here, we report for the first time on the MBE-grown TMD exhibiting narrow and resolved spectral lines of neutral and charged exciton. Moreover, our material exhibits unprecedented high homogeneity of optical properties, with variation of the exciton energy as small as ±0.16 meV over a distance of tens of micrometers. Our recipe for MBE growth is presented for MoSe2and includes the use of atomically flat hexagonal boron nitride substrate. This recipe opens a possibility of producing TMD heterostructures with optical quality, dimensions, and homogeneity required for optoelectronic applications.

We found that optical Aharonov–Bohm oscillations in a single GaAs/GaAlAs quantum ring can be controlled by excitation intensity. With a weak excitation intensity of 1.2 kW cm–2, the optical Aharonov–Bohm oscillation period of biexcitons was observed to be half that of excitons in accordance with the period expected for a two-exciton Wigner molecule. When the excitation intensity is increased by an order of magnitude (12 kW cm–2), a gradual deviation of the Wigner molecule condition occurs with decreased oscillation periods and diamagnetic coefficients for both excitons and biexcitons along with a spectral shift. These results suggest that the effective orbit radii and rim widths of electrons and holes in a single quantum ring can be modified by light intensity via photoexcited carriers, which are possibly trapped at interface defects resulting in a local electric field.

Recent results on the optical properties of monolayer and few layers of semiconducting transition metal dichalcogenides are reviewed. Experimental observations are presented and discussed in the frame of existing models, highlighting the limits of our understanding in this emerging field of research. We first introduce the representative band structure of these systems and their interband optical transitions. The effect of an external magnetic field is then considered to discuss Zeeman spectroscopy and optical pumping experiments, both revealing phenomena related to the valley degree of freedom. Finally, we discuss the observation of single photon emitters in different types of layered materials, including wide band gap hexagonal boron nitride. While going through these topics, we try to focus on open questions and on experimental observations, which do not yet have a clear explanation.

Temperature-dependent (5 K–300 K) Raman scattering study of A1g/A′1phonon modes in mono-layer (1L), bilayer (2L), trilayer (3L), and tetralayer (4L) MoTe2is reported. The temperature evolution of the modes’ intensity critically depends on the flake thickness. In particular with λ=632.8-nm light excitation, a strongly non-monotonic dependence of the A1gmode intensity is observed in 2L MoTe2. The intensity decreases with decreasing temperature down to 220 K, and the A1gmode almost completely vanishes from the Stokes scattering spectrum in the temperature range between 160 K and 220 K. The peak recovers at lower temperatures, and at T=5 K, it becomes three times more intense that at room temperature. Similar non-monotonic intensity evolution is observed for the out-of-plane mode in 3L MoTe2in which tellurium atoms in all three layers vibrate in-phase. The intensity of the other out-of-plane Raman-active mode (with vibrations of tellurium atoms in the central layer shifted by 180° with respect to the vibrations in outer layers) only weakly depends on temperature. The observed quenching of the Raman scattering in 2L and 3L MoTe2is attributed to a destructive interference between the resonant and non-resonant contributions to the Raman scattering amplitude. The observed “antiresonance” is related to the electronic excitation at the M point of the Brillouin zone in few-layer MoTe2.

Magnetic layered materials have emerged recently as promising systems to introduce magnetism in structures based on two-dimensional (2D) materials and to investigate exotic magnetic ground states in the 2D limit. In this work, we apply high hydrostatic pressures up to P≈ 8.7 GPa to the bulk layered antiferromagnet FePS3to tune the collective lattice excitations (phonons) in resonance with magnetic excitations (magnons). Close to P= 4 GPa, the magnon-phonon resonance is achieved, and the strong coupling between these collective modes leads to the formation of new quasiparticles, the magnon-polarons, evidenced in our low-temperature Raman scattering experiments by a particular avoided crossing behavior between the phonon and the doubly degenerate antiferromagnetic magnon. At the pressure-induced magnon-phonon resonance, three distinct coupled modes emerge. As it is mainly defined by intralayer properties, we show that the energy of the magnon is nearly pressure-independent. We additionally apply high magnetic fields up to B= 30 T to fully identify and characterize the magnon excitations and to explore the different magnon-polaron regimes for which the phonon has an energy lower than, equal to, or higher than the magnon energy. The description of our experimental data requires introducing a phonon-phonon coupling not taken into account in actual calculations.

We report interband circularly polarized magneto-photoluminescence results for In0.53Ga0.47As quantum wires of various widths in magnetic fields up to 28 T. The experimental results reveal a highly wire width dependent Zeeman splitting compared to the quantum well reference and even a reversal of the Zeeman split transitions arising from the lowest conduction and valence states in the quantum wires. The total g-factor, g=ge+gv, is therefore highly wire width dependent.