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Register a new userPopulation pulsation resonances of excitons in monolayer MoSe2 with sub 1 {mu}eV linewidth
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Monolayer transition metal dichalcogenides, a new class of atomically thin semiconductors, possess optically coupled 2D valley excitons. The nature of exciton relaxation in these systems is currently poorly understood. Here, we investigate exciton relaxation in monolayer MoSe2 using polarization-resolved coherent nonlinear optical spectroscopy with high spectral resolution. We report strikingly narrow population pulsation resonances with two different characteristic linewidths of 1 {mu}eV and <0.2 {mu}eV at low-temperature. These linewidths are more than three orders of magnitude narrower than the photoluminescence and absorption linewidth, and indicate that a component of the exciton relaxation dynamics occurs on timescales longer than 1 ns. The ultra-narrow resonance (<0.2 {mu}eV) emerges with increasing excitation intensity, and implies the existence of a long-lived state whose lifetime exceeds 6 ns.
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We report on high frequency resolution coherent nonlinear optical spectroscopy on an ensemble of InGaN disks in GaN nanowires at 300 K. Sub-$mu$eV resonances in the inhomogeneously broadened third order ($chi^{(3)}$) absorption spectrum show asymmetric line shapes, where the degree of asymmetry depends on the wavelength of the excitation beams. Theory based on the Optical Bloch Equations (OBE) indicates that the lineshape asymmetry is a result of fast decoherence in the system and the narrow resonances originate from coherent population pulsations that are induced by decoherence in the system. Using the OBE, we estimate that the decoherence time of the optically induced dipole (formed between the unexcited ground state the excited electron-hole pair) at room temperature is 125 fs, corresponding to a linewidth of ~10 meV. The decay time of the excitation is ~5-10 ns, depending on the excitation energy. The lineshapes are well fit with the OBE indicating that the resonances are characterized by discrete levels with no evidence of many body physics.
Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, with bound electrons and holes localized in individual monolayers, i.e. interlayer excitons. Here, we report the first observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by both photoluminescence and photoluminescence excitation spectroscopy. The energy and luminescence intensity of interlayer excitons are highly tunable by an applied vertical gate voltage, implying electrical control of the heterojunction band-alignment. Using time resolved photoluminescence, we find that the interlayer exciton is long-lived with a lifetime of about 1.8 ns, an order of magnitude longer than intralayer excitons13-16. Our work demonstrates the ability to optically pump interlayer electric polarization and provokes the immediate exploration of interlayer excitons for condensation phenomena, as well as new applications in 2D light-emitting diodes, lasers, and photovoltaic devices.
Monolayers of semiconducting transition metal dichalcogenides (TMDCs) with unique spin-valley contrasting properties and remarkably strong excitonic effects continue to be a subject of intense research interests. These model 2D semiconductors feature two fundamental intravalley excitons species - optically accessible bright excitons with anti-parallel spins and optically inactive dark excitons with parallel spins. For applications exploiting radiative recombination of bright excitons or long lifetime dark excitons, it is essential to understand the radiative character of the exciton ground state and establish the energy separation between the lowest energy bright and dark excitons. Here, we report a direct spectroscopic measure of dark excitons in monolayer MoSe$_2$ encapsulated in hexagonal boron nitride. By applying strong in-plane magnetic field, we induce mixing and splitting of bright and dark exciton branches, which enables an accurate spectroscopic determination of their energies. We confirm the bright character of the exciton ground state separated by a 1.5~meV gap from the higher energy dark exciton state, much smaller compared to the previous theoretical expectations. These findings provide critical information for further improvement of the accurate theoretical description of TMDCs electronic structure.
We observe unusually narrow donor-bound exciton transitions (0.4 meV) in the photoluminescence spectra of GaN nanowire ensembles grown on Si(111) substrates at very high (> 850 degrees Celsius) temperatures. The spectra of these samples reveal a prominent transition of excitons bound to neutral Si impurities which is not observed for samples grown under standard conditions. Motivated by these experimental results, we investigate theoretically the impact of surface-induced internal electric fields on the binding energy of donors by a combined Monte Carlo and envelope function approach. We obtain the ranges of doping and diameter for which the potential is well described using the Poisson equation, where one assumes a spatially homogeneous distribution of dopants. Our calculations also show that surface donors in nanowires with a diameter smaller than 100 nm are ionized when the surface electric field is larger than about 10 kV/cm, corresponding to a doping level higher than 2 x 10^16 cm^-3. This result explains the experimental observation: since the (D+,X) complex is not stable in GaN, surface-donor-bound excitons do not contribute to the photoluminescence spectra of GaN nanowires above a certain doping level, and the linewidth reflects the actual structural perfection of the nanowire ensemble.
Monolayer transition metal dichalcogenide semiconductors, with versatile experimentally accessible exciton species, offer an interesting platform for investigating the interaction between excitons and a Fermi sea of charges. Using hexagonal boron nitride encapsulated monolayer MoSe2, we study the impact of charge density tuning on the ground and excited Rydberg states in the atomic layer. Consistent excitonpolaron behavior is revealed in both photoluminescence and reflection spectra of the A exciton 1s (A:1s) Rydberg state, in contrast to previous studies. The A:2s Rydberg state provides an opportunity to understand such interactions with greatly reduced exciton binding energy. We found that the impact of the Fermi sea becomes much more dramatic. With a photoluminescence upconversion technique, we further verify the 2s polaron-like behavior for the repulsive branch of B:2s exciton whose energy is well above the bare bandgap. Our studies show that the polaron-like interaction features are quite generic and highly robust, offering key insights into the dressed manybody state in a Fermi sea.
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