Spatiotemporal dynamics of photoexcited quasiparticles in two-dimensional crystals studied by ultrafast laser techniques

Layered materials in which atomic sheets are stacked together by weak van der Waals forces can be used to fabricate two-dimensional systems. They represent a diverse and rich, but largely unexplored, source of materials. Atomically-thin structures derived from these materials possess a number of interesting electrical, optical, and mechanical properties, and are attractive for new nanodevices. For their applications in semiconductor industry, it is necessary to understand the dynamics of photoexcited quasiparticles that occur on ultrafast time scales of less than one nanosecond. In this dissertation, I discuss ultrafast optical experimental techniques and results from various two-dimensional materials, which provide information about electronic dynamics. First, a second harmonic generation technique that can be used to find the crystalline orientation, thickness uniformity, layer stacking, and single-crystal domain size is discussed, with results presented on exfoliated and chemical vapor deposition MoS2 samples. Second, a third harmonic generation technique is discussed, which can be used to explore nonlinear optical properties of materials, and results are presented on graphene and few-layer graphite films. Third, a spatially resolved femtosecond pump-probe is described, which can be used to study hot carrier and photoexcited phonon dynamics and results are presented on Bi2 Se3 sample. Then, exciton dynamics in MoS2 and MoSe2 are explored by using transient absorption microscopy with a high spatiotemporal resolution. Finally, a polarization-resolved femtosecond transient absorption spectroscopy that can be used to study valley and spin dynamics is discussed, with results presented on monolayer, few-layer, and bulk MoSe2 samples

Exciton-exciton annihilation in MoSe2 monolayers

We investigate the excitonic dynamics in MoSe2 monolayer and bulk samples by femtosecond transient absorption microscopy. Excitons are resonantly injected by a 750-nm and 100-fs laser pulse, and are detected by a probe pulse tuned in the range of 790 - 820 nm. We observe a strong density-dependent initial decay of the exciton population in monolayers, which can be well described by the exciton-exciton annihilation. Such a feature is not observed in the bulk under comparable conditions. We also observe the saturated absorption induced by exciton phase-space filling in both monolayers and the bulk, which indicates their potential applications as saturable absorbers.Comment: 5 pages, 4 figure

Two-probe study of hot carriers in reduced graphene oxide

The energy relaxation of carriers in reduced graphene oxide thin films is studied using optical pump-probe spectroscopy with two probes of different colors. We measure the time difference between peaks of the carrier density at each probing energy by measuring a time-resolved differential transmission and find that the carrier density at the lower probing energy peaks later than that at the higher probing energy. Also, we find that the peak time for the lower probing energy shifts from about 92 to 37 fs after the higher probing energy peak as the carrier density is increased from 1.5E12 to 3E13 per square centimeter, while no noticeable shift is observed in that for the higher probing energy. Assuming the carriers rapidly thermalize after excitation, this indicates that the optical phonon emission time decreases from about 50 to about 20 fs and the energy relaxation rate increases from 4 to 10 meV/fs. The observed density dependence is inconsistent with the phonon bottleneck effect.Comment: 10 pages, 4 figure

Tightly bound excitons in monolayer WSe2

Exciton binding energy and excited states in monolayers of tungsten diselenide (WSe2) are investigated using the combined linear absorption and two-photon photoluminescence excitation spectroscopy. The exciton binding energy is determined to be 0.37eV, which is about an order of magnitude larger than that in III-V semiconductor quantum wells and renders the exciton excited states observable even at room temperature. The exciton excitation spectrum with both experimentally determined one- and two-photon active states is distinct from the simple two-dimensional (2D) hydrogenic model. This result reveals significantly reduced and nonlocal dielectric screening of Coulomb interactions in 2D semiconductors. The observed large exciton binding energy will also have a significant impact on next-generation photonics and optoelectronics applications based on 2D atomic crystals.Comment: 19 pages, 4 figures, to appear in PR

Spatially resolved femtosecond pump-probe study of topological insulator Bi2Se3

Carrier and phonon dynamics in Bi2Se3 crystals are studied by a spatially resolved ultrafast pump-probe technique. Pronounced oscillations in differential reflection are observed with two distinct frequencies, and are attributed to coherent optical and acoustic phonons, respectively. The rising time of the signal indicates that the thermalization and energy relaxation of hot carriers are both sub-ps in this material. We found that the thermalization and relaxation time decreases with the carrier density. The expansion of the differential reflection profile allows us to estimate an ambipolar carrier diffusion coefficient on the order of 500 square centimeters per second. A long-term slow expansion of the profile shows a thermal diffusion coefficient of 1.2 square centimeters per second.Comment: 8 pages, 6 figure

Second harmonic microscopy of monolayer MoS2

We show that the lack of inversion symmetry in monolayer MoS2 allows strong optical second harmonic generation. Second harmonic of an 810-nm pulse is generated in a mechanically exfoliated monolayer, with a nonlinear susceptibility on the order of 1E-7 m/V. The susceptibility reduces by a factor of seven in trilayers, and by about two orders of magnitude in even layers. A proof-of-principle second harmonic microscopy measurement is performed on samples grown by chemical vapor deposition, which illustrates potential applications of this effect in fast and non-invasive detection of crystalline orientation, thickness uniformity, layer stacking, and single-crystal domain size of atomically thin films of MoS2 and similar materials.Comment: 6 pages, 4 figure

Ionic-passivated FeS2 photocapacitors for energy conversion and storage

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