Magnon gap excitations in van der Waals antiferromagnet MnPSe.

Magneto-spectroscopy methods have been employed to study the zero-wavevector magnon excitations in MnPSe. Experiments carried out as a function of temperature and the applied magnetic field show that two low-energy magnon branches of MnPSe in its antiferromagnetic phase are gapped. The observation of two low-energy magnon gaps (at 1.

Magneto-Optical Sensing of the Pressure Driven Magnetic Ground States in Bulk CrSBr.

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.

High-Angular Momentum Excitations in Collinear Antiferromagnet FePS.

We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS. 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 || = 4 multipolar magnon─a single-ion 4-magnon bound state─that corresponds to a full reversal of a single magnetic moment of the Fe ion.

High-Pressure Tuning of Magnon-Polarons in the Layered Antiferromagnet FePS.

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 ≈ 8.7 GPa to the bulk layered antiferromagnet FePS to tune the collective lattice excitations (phonons) in resonance with magnetic excitations (magnons).

Spatially resolved optical spectroscopy in extreme environment of low temperature, high magnetic fields and high pressure.

We present an experimental setup developed to perform optical spectroscopy experiments (Raman scattering and photoluminescence measurements) with a micrometer spatial resolution in an extreme environment of low temperature, high magnetic field, and high pressure. This unique experimental setup, to the best of our knowledge, allows us to deeply explore the phase diagram of condensed matter systems by independently tuning these three thermodynamic parameters while monitoring the low-energy excitations (electronic, phononic, or magnetic excitations) to spatially map the Raman scattering response or to investigate objects with low dimensions. We apply this technique to bulk FePS, a layered antiferromagnet with a Néel temperature of T ≈ 120 K.

Manganese doping for enhanced magnetic brightening and circular polarization control of dark excitons in paramagnetic layered hybrid metal-halide perovskites.

Materials combining semiconductor functionalities with spin control are desired for the advancement of quantum technologies. Here, we study the magneto-optical properties of novel paramagnetic Ruddlesden-Popper hybrid perovskites Mn:(PEA)PbI (PEA = phenethylammonium) and report magnetically brightened excitonic luminescence with strong circular polarization from the interaction with isolated Mn ions. Using a combination of superconducting quantum interference device (SQUID) magnetometry, magneto-absorption and transient optical spectroscopy, we find that a dark exciton population is brightened by state mixing with the bright excitons in the presence of a magnetic field.

Excitonic Complexes in n-Doped WS Monolayer.

We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of n-doped WS monolayer 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.

Neutral and charged dark excitons in monolayer WS.

Low temperature and polarization resolved magneto-photoluminescence experiments are used to investigate the properties of dark excitons and dark trions in a monolayer of WS2 encapsulated in hexagonal BN (hBN). We find that this system is an n-type doped semiconductor and that dark trions dominate the emission spectrum. In line with previous studies on WSe2, we identify the Coulomb exchange interaction coupled neutral dark and grey excitons through their polarization properties, while an analogous effect is not observed for dark trions.

Valley polarization of singlet and triplet trions in a WS monolayer in magnetic fields.

The spectral signatures associated with different negatively charged exciton complexes (trions) in a WS2 monolayer encapsulated in hBN are analyzed from low temperature and polarization resolved reflectance contrast (RC) and photoluminescence (PL) experiments, with an applied magnetic field. Based on results obtained from the RC experiment, we show that the valley Zeeman effect affects the optical response of both the singlet and the triplet trion species through the evolution of their energy and of their relative intensity, when applying an external magnetic field. Our analysis allows us to estimate a free electron concentration of ∼1.

Measurement of the spin-forbidden dark excitons in MoS and MoSe monolayers.

Excitons with binding energies of a few hundreds of meV control the optical properties of transition metal dichalcogenide monolayers. Knowledge of the fine structure of these excitons is therefore essential to understand the optoelectronic properties of these 2D materials. Here we measure the exciton fine structure of MoS and MoSe monolayers encapsulated in boron nitride by magneto-photoluminescence spectroscopy in magnetic fields up to 30 T.

Magnon bound states versus anyonic Majorana excitations in the Kitaev honeycomb magnet α-RuCl.

The pure Kitaev honeycomb model harbors a quantum spin liquid in zero magnetic fields, while applying finite magnetic fields induces a topological spin liquid with non-Abelian anyonic excitations. This latter phase has been much sought after in Kitaev candidate materials, such as α-RuCl. Currently, two competing scenarios exist for the intermediate field phase of this compound (B = 7 - 10 T), based on experimental as well as theoretical results: (i) conventional multiparticle magnetic excitations of integer quantum number vs.

The effect of metallic substrates on the optical properties of monolayer MoSe.

Atomically thin materials, like semiconducting transition metal dichalcogenides (S-TMDs), are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. Photoluminescence and reflectance contrast techniques are employed to investigate the effect of metallic substrates on optical properties of MoSe monolayer (ML).

Energy Spectrum of Two-Dimensional Excitons in a Nonuniform Dielectric Medium.

We demonstrate that, in monolayers (MLs) of semiconducting transition metal dichalcogenides, the s-type Rydberg series of excitonic states follows a simple energy ladder: ε_{n}=-Ry^{*}/(n+δ)^{2}, n=1,2,…, in which Ry^{*} is very close to the Rydberg energy scaled by the dielectric constant of the medium surrounding the ML and by the reduced effective electron-hole mass, whereas the ML polarizability is accounted for only by δ. This is justified by the analysis of experimental data on excitonic resonances, as extracted from magneto-optical measurements of a high-quality WSe_{2} ML encapsulated in hexagonal boron nitride (hBN), and well reproduced with an analytically solvable Schrödinger equation when approximating the electron-hole potential in the form of a modified Kratzer potential. Applying our convention to other MoSe_{2}, WS_{2}, MoS_{2} MLs encapsulated in hBN, we estimate an apparent magnitude of δ for each of the studied structures.

Probing and Manipulating Valley Coherence of Dark Excitons in Monolayer WSe_{2}.

Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX_{2} (X being S or Se) spin forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe_{2} monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsic exchange interaction in combination with the applied in-plane and/or out-of-plane magnetic fields enables one to probe and manipulate the valley degree of freedom of the dark excitons.

Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures.

The intriguing physics of carrier-carrier interactions, which likewise affect the operation of light emitting devices, stimulate the research on semiconductor structures at high densities of excited carriers, a limit reachable at large pumping rates or in systems with long-lived electron-hole pairs. By electrically injecting carriers into WSe/MoS type-II heterostructures which are indirect in real and k-space, we establish a large population of typical optically silent interlayer excitons. Here, we reveal their emission spectra and show that the emission energy is tunable by an applied electric field.

The lifetime of interlayer breathing modes of few-layer 2H-MoSe membranes.

A time-resolved observation of coherent interlayer longitudinal acoustic phonons in thin layers of 2H-MoSe2 is reported. A femtosecond pump-probe technique is used to investigate the evolution of the energy loss of these vibrational modes in a wide selection of MoSe2 flakes with different thicknesses ranging from bilayer up to the bulk limit. By directly analysing the temporal decay of the modes, we can clearly distinguish an abrupt crossover related to the acoustic mean free path of the phonons in a layered system, and the constraints imposed on the acoustic decay channels when reducing the dimensionality.

Singlet and triplet trions in WS monolayer encapsulated in hexagonal boron nitride.

Embedding a WS monolayer in flakes of hexagonal boron nitride allowed us to resolve and study the photoluminescence response due to both singlet and triplet states of negatively charged excitons (trions) in this atomically thin semiconductor. The energy separation between the singlet and triplet states has been found to be relatively small reflecting rather weak effects of the electron-electron exchange interaction for the trion triplet in a WS monolayer, which involves two electrons with the same spin but from different valleys. Polarization-resolved experiments demonstrate that the helicity of the excitation light is better preserved in the emission spectrum of the triplet trion than in that of the singlet trion.

Magneto-absorption spectra of hydrogen-like yellow exciton series in cuprous oxide: excitons in strong magnetic fields.

We study the absorption spectra of the yellow excitons in CuO in high magnetic fields using polarization-resolved optical absorption measurements with a high frequency resolution. We show that the symmetry of the yellow exciton results in unusual selection rules for the optical absorption of polarized light and that the mixing of ortho- and para- excitons in magnetic field is important. The calculation of the energies of the yellow exciton series in strong and weak magnetic field limits suggests that a broad n = 2 line is comprized by two closely overlapping lines, gives a good fit to experimental data and allows to interpret the complex structure of excitonic levels.

Sub-bandgap Voltage Electroluminescence and Magneto-oscillations in a WSe Light-Emitting van der Waals Heterostructure.

We report on experimental investigations of an electrically driven WSe based light-emitting van der Waals heterostructure. We observe a threshold voltage for electroluminescence significantly lower than the corresponding single particle band gap of monolayer WSe. This observation can be interpreted by considering the Coulomb interaction and a tunneling process involving excitons, well beyond the picture of independent charge carriers.

Magneto-Optical Signature of Massless Kane Electrons in Cd_{3}As_{2}.

We report on optical reflectivity experiments performed on Cd_{3}As_{2} over a broad range of photon energies and magnetic fields. The observed response clearly indicates the presence of 3D massless charge carriers. The specific cyclotron resonance absorption in the quantum limit implies that we are probing massless Kane electrons rather than symmetry-protected 3D Dirac particles.

Radiatively Limited Dephasing and Exciton Dynamics in MoSe2 Monolayers Revealed with Four-Wave Mixing Microscopy.

By implementing four-wave mixing (FWM) microspectroscopy, we measure coherence and population dynamics of the exciton transitions in monolayers of MoSe2. We reveal their dephasing times T2 and radiative lifetime T1 in a subpicosecond (ps) range, approaching T2 = 2T1 and thus indicating radiatively limited dephasing at a temperature of 6 K. We elucidate the dephasing mechanisms by varying the temperature and by probing various locations on the flake exhibiting a different local disorder.

Rhombohedral Multilayer Graphene: A Magneto-Raman Scattering Study.

Graphene layers are known to stack in two stable configurations, namely, ABA or ABC stacking, with drastically distinct electronic properties. Unlike the ABA stacking, little has been done to experimentally investigate the electronic properties of ABC graphene multilayers. Here, we report on the first magneto optical study of a large ABC domain in a graphene multilayer flake, with ABC sequences exceeding 17 graphene sheets.

Micro-Raman and infrared studies of multiferroic TbMn₂O₅.

We have studied the Raman and infrared spectral response of TbMn2O5 under an applied magnetic field parallel to the easy magnetic a-axis at 4.2 K. Strong spin-lattice coupling in TbMn2O5 is evidenced by a frequency shift of Raman and infrared phonons as a function of magnetic field compared to the phonon response of BiMn2O5 that remains unaffected.

Strong interband Faraday rotation in 3D topological insulator Bi2Se3.

The Faraday effect is a representative magneto-optical phenomenon, resulting from the transfer of angular momentum between interacting light and matter in which time-reversal symmetry has been broken by an externally applied magnetic field. Here we report on the Faraday rotation induced in the prominent 3D topological insulator Bi2Se3 due to bulk interband excitations. The origin of this non-resonant effect, extraordinarily strong among other non-magnetic materials, is traced back to the specific Dirac-type Hamiltonian for Bi2Se3, which implies that electrons and holes in this material closely resemble relativistic particles with a non-zero rest mass.