Breaking space-time symmetries in two-dimensional crystals can markedly influence their macroscopic electronic properties. Monolayer transition metal dichalcogenides (TMDs) are prime examples where the intrinsically broken crystal inversion symmetry permits the generation of valley-selective electron populations, even though the two valleys are energetically degenerate, locked by time-reversal symmetry. Lifting the valley degeneracy in these materials is of great interest because it would allow for valley-specific band engineering and offer additional control in valleytronic applications. Although applying a magnetic field should, in principle, accomplish this task, experiments so far have not shown valley-selective energy level shifts in fields accessible in the laboratory. Here, we show the first direct evidence of lifted valley degeneracy in the monolayer TMD WS2. By applying intense circularly polarized light, which breaks time-reversal symmetry, we demonstrate that the exciton level in each valley can be selectively tuned by as much as 18 meV through the optical Stark effect. These results offer a new way to control the valley degree of freedom, and may provide a means to realize new Floquet topological phases in two-dimensional TMDs.
We perform time- and angle-resolved photoemission spectroscopy of a prototypical topological insulator (TI) Bi(2)Se(3) to study the ultrafast dynamics of surface and bulk electrons after photoexcitation. By analyzing the evolution of surface states and bulk band spectra, we obtain their electronic temperature and chemical potential relaxation dynamics separately. These dynamics reveal strong phonon-assisted surface-bulk coupling at high lattice temperature and total suppression of inelastic scattering between the surface and the bulk at low lattice temperature. In this low temperature regime, the unique cooling of Dirac fermions in TI by acoustic phonons is manifested through a power law dependence of the surface temperature decay rate on carrier density.
The author observe sixfold enhancement in the near band gap emission of ZnO nanorods by employing surface plasmon of Au nanoparticles, while the defect-related emission is completely suppressed. Time-resolved photoluminescence indicates that the decay process becomes much faster by Au capping. The remarkable enhancement of the ultraviolet emission intensities and transition rates is ascribed to the charge transfer and efficient coupling between ZnO nanorods and Au surface plasmons. The suppression of the green emission might be due to a combined effect of Au surface plasmon and passivation of the ZnO nanorod surface traps.
When electrons in a solid are excited with light, they can alter the free energy landscape and access phases of matter that are beyond reach in thermal equilibrium. This accessibility becomes of vast importance in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by light. Here, we study a layered compound, LaTe3, where a small in-plane (a-c plane) lattice anisotropy results in a unidirectional charge density wave (CDW) along the c-axis. Using ultrafast electron diffraction, we find that after photoexcitation, the CDW along the c-axis is weakened and subsequently, a different competing CDW along the a-axis emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for unleashing similar states of matter that are "trapped" under equilibrium conditions.
Interactions between two excitons can result in the formation of bound quasiparticles, known as biexcitons. Their properties are determined by the constituent excitons, with orbital and spin states resembling those of atoms. Monolayer transition metal dichalcogenides (TMDs) present a unique system where excitons acquire a new degree of freedom, the valley pseudospin, from which a novel intervalley biexciton can be created. These biexcitons comprise two excitons from different valleys, which are distinct from biexcitons in conventional semiconductors and have no direct analogue in atomic and molecular systems. However, their valley properties are not accessible to traditional transport and optical measurements. Here, we report the observation of intervalley biexcitons in the monolayer TMD MoS2 using ultrafast pump-probe spectroscopy. By applying broadband probe pulses with different helicities, we identify two species of intervalley biexcitons with large binding energies of 60 meV and 40 meV. In addition, we also reveal effects beyond biexcitonic pairwise interactions in which the exciton energy redshifts at increasing exciton densities, indicating the presence of many-body interactions among them.
Intrinsic defects such as vacancies, interstitials, and anti-sites often introduce rich luminescent properties in II-VI semiconductor nanomaterials. A clear understanding of the dynamics of the defect-related excitons is particularly important for the design and optimization of nanoscale optoelectronic devices. In this paper, low-temperature steady-state and time-resolved photoluminescence (PL) spectroscopies have been carried out to investigate the emission of cadmium sulfide (CdS) nanobelts that originates from the radiative recombination of excitons bound to neutral donors (I(2)) and the spatially localized donor-acceptor pairs (DAP), in which the assignment is supported by first principle calculations. Our results verify that the shallow donors in CdS are contributed by sulfur vacancies while the acceptors are contributed by cadmium vacancies. At high excitation intensities, the DAP emission saturates and the PL is dominated by I(2) emission. Beyond a threshold power of approximately 5 μW, amplified spontaneous emission (ASE) of I(2) occurs. Further analysis shows that these intrinsic defects created long-lived (spin triplet) DAP trap states due to spin-polarized Cd vacancies which become saturated at intense carrier excitations.
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