Hydrostatic pressure effect of photocarrier dynamics in GaAs probed by time-resolved terahertz spectroscopy.

Pressure effects on photocarrier dynamics such as interband relaxations and intraband cooling in GaAs have been investigated using in situ time-resolved terahertz spectroscopy with a diamond anvil cell. The interband photocarrier lifetime significantly decreases by nearly two orders of magnitude as the external hydrostatic pressure is increased up to 10 GPa. Considerable pressure tuning for the intervalley scattering processes has also been observed, and the time constants under different pressures are extracted based on the three-state rate model. This work provides new perspectives on tailoring nonequilibrium carrier dynamics in semiconductors using hydrostatic pressure and may serve as the impetus for the development of high-pressure terahertz spectroscopy.

Transient photoconductivity and free carrier dynamics in a monolayer WS2 probed by time resolved Terahertz spectroscopy.

The frequency and time resolved conductivity in a photoexcited large-area monolayer tungsten disulfide (WS2) have been simultaneously determined by using time-resolved terahertz spectroscopy. We use the Drude-Smith model to successfully reproduce the transient photoconductivity spectra, which demonstrate that localized free carriers, not bounded excitons, are responsible for the THz transport. Upon the optical excitation with 400 nm and 530 nm wavelength, the relaxation dynamics of the free carriers include fast and slow decay components with time constants approximately smaller than 1 ps and between 5-7 ps, respectively. The former sub-picosecond decay is attributed to the charge carrier loss induced by the exciton formation, while both the Auger recombination and the surface trapping can contribute to the slow relaxation.

Pressure-Induced Bifurcation in the Photoluminescence of Red Carbon Quantum Dots: Coexistence of Emissions from Surface Groups and Nitrogen-Doped Cores.

Carbon quantum dots (CDs) with favorable fluorescent properties have stimulated considerable effort to modulate their photoluminescence (PL) for bioimaging and sensing. However, the fluorescent mechanisms are still only partially understood due to the diverse physicochemical properties of CDs prepared by various synthesis methods and postpreparation processes. In this report, pressure-induced bifurcation of PL is reported in red carbon quantum dots (R-CDs) for the first time. The splitting of PL into an irreversible blue-shifted peak and a reversible red-shifted peak under pressure suggests the coexistence of multiple fluorescent mechanisms in R-CDs, i.e., emissions from surface groups and nitrogen-doped cores. The concentration and excitation laser energy dependencies of pressure-induced bifurcation, as well as the time-resolved PL, further support the coexistence of multiple emitters. Our results provide a method for distinguishing between the different fluorescent mechanisms related to surface groups and carbon cores in CDs.

High-Pressure Insertion of Dense H2 into a Model Zeolite.

Our combined high-pressure synchrotron X-ray diffraction and Monte Carlo modeling studies show super-filling of the zeolite, and computational results suggest an occupancy by a maximum of nearly two inserted H2 molecules per framework unit, which is about twice that observed in gas hydrates. Super-filling prevents amorphization of the host material up to at least 60 GPa, which is a record pressure for zeolites and also for any group IV element being in full 4-fold coordination, except for carbon. We find that the inserted H2 forms an exotic topologically constrained glassy-like form, otherwise unattainable in pure hydrogen. Raman spectroscopy on confined H2 shows that the microporosity of the zeolite is retained over the entire investigated pressure range (up to 80 GPa) and that intermolecular interactions share common aspects with bulk hydrogen, while they are also affected by the zeolite framework.

Identifying the Intermediate Free-Carrier Dynamics Across the Charge Separation in Monolayer MoS2/ReSe2 Heterostructures.

Van der Waals heterostructures composed of different two-dimensional films offer a unique platform for engineering and promoting photoelectric performances, which highly demands the understanding of photocarrier dynamics. Herein, large-scale vertically stacked heterostructures with MoS2 and ReSe2 monolayers are fabricated. Correspondingly, the carrier dynamics have been thoroughly investigated using different ultrafast spectroscopies, including Terahertz (THz) emission spectroscopy, time-resolved THz spectroscopy (TRTS), and near-infrared optical pump-probe spectroscopy (OPPS), providing complementary dynamic information for the out-of-plane charge separation and in-plane charge transport at different stages. The initial charge transfer (CT) within the first 170 fs, generating a transient directional current, is directly demonstrated by the THz emissions. Furthermore, the TRTS explicitly unveils an intermediate free-carrier relaxation pathway, featuring a pronounced augmentation of THz photoconductivity compared to the isolated ReSe2 layer, which likely contains the evolution from immigrant hot charged free carriers to bounded interlayer excitons (∼0.7 ps) and the surface defect trapping (∼13 ps). In addition, the OPPS reveals a distinct enhancement in the saturable absorption along with long-lived dynamics (∼365 ps), which originated from the CT and interlayer exciton recombination. Our work provides comprehensive insight into the photocarrier dynamics across the charge separation and will help with the development of optoelectronic devices based on ReSe2-MoS2 heterostructures.