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We investigated ultrafast defect-lattice dynamics in diamond using the N_s:±á−C⁰ defect, an analog of bond-centered hydrogen in semiconductors. Combining synthesis, ultrafast vibrational spectroscopy, and ab initio calculations, we show that excitation of the defect’s stretch mode leads to the generation of localized phonons and the formation of a hot ground state, where the interatomic potential is transiently modified. Our results reveal unexpected nonequilibrium phonon effects despite diamond’s exceptionally high thermal conductivity, with implications for quantum defect engineering.

We report on the terahertz (THz) harmonic generation in an active graphene/metamaterial device by using powerful ultrafast table-top THz time-domain spectroscopic systems. Complex nonlinear transmission spectra, comprising even and odd harmonics, emerge when the devices are tested with intense ultrafast THz pulses with peak electric fields in the range of 1–150 kV/cm. The odd and even harmonic features show a positive correlation with carrier concentration, allowing for efficient frequency tuning on top of tunable group delay dispersion. Interestingly, before the onset of saturation, observed at 20–25 kV/cm, the main resonance and the harmonic features exhibit an anti-crossing trend that can be further exploited for active frequency tuning. These results report a key milestone for the fundamental investigation of the nonlinearity of 2D materials. At the same time, they represent an important advance in the design of future integrated THz optoelectronics by providing novel functionalities for THz light generation and manipulation.

Monolayer molybdenum disulfide (1L MoS2), a promising optoelectronic material, emits strong visible photoluminescence (PL). Systematic control of the intensity, energy, and spectral width of PL from 1L MoS2 on silicon dioxide/silicon (SiO2/Si) is demonstrated via simple external treatments. Treating MoS2 with solutions formed from the superacid bis-(trifluoromethanesulfonyl)amide (TFSA) enhances, blueshifts, and sharpens the PL. Treatments with solutions from structurally analogous chemicals that lack sulfur, in the case of bis(trifluoroacetamide) (BTFA), or lack fluorine, in the case of methanesulfonamide (MSA), show the same trend, suggesting a two-component mechanism for TFSA involving the presence of electronegative species and sulfur vacancy passivation. Up to ≈100× enhancement of the PL intensity is achieved, with the peak blueshifted by ≈30 meV and the spectral linewidth halved. Conversely, direct thermal atomic layer deposition (ALD) of aluminum oxide (Al2O3) or hafnium oxide (HfO2) is found to suppress the PL by up to a factor of ≈3, redshift by up to ≈70 meV, and broaden by ≈3×. Single-spot and mapping Raman/PL techniques are combined in a robust characterization process to associate changes in the PL character to charge doping. This work demonstrates the convenient tunability of the optical behavior of 1L MoS2 by varying the electron density.

Layered hybrid perovskites (LPKs) are promising as alternatives or additives to 3D metal halide perovskites for optoelectronic applications including photovoltaic cells, LEDs and lasers due to their increased stability. However, high exciton binding energies in these materials mean that excitons are the majority species under the operating conditions of many devices. Although the efficiency of devices that incorporate LPKs has been increasing, much is still unknown about the interplay of excitons and free charge-carriers in these materials, which is vital information for understanding how optoelectronic properties dictate device efficiency. In this work, we employ optical pump/THz probe spectroscopy (OPTP) and visible transient absorption spectroscopy (TAS) to analyse the optoelectronic properties and charge-carrier dynamics of phenylethylammonium lead iodide (PEA)2PbI4. By combining these techniques, we are able to disentangle the contributions from excitons and free charge-carriers. We observe fast cooling of free charge-carriers and exciton formation on a timescale of ∼400 fs followed by slower bimolecular recombination of residual free charge-carriers with a rate constant k2 ∼ 109 cm3s−1. Excitons recombine via two monomolecular processes with lifetimes t1 ∼ 11 ps and t2 ∼ 83 ps. Furthermore, we detect signatures of exciton–phonon coupling in the transient absorption kinetic traces. These findings provide new insight into the interplay between free charge-carriers and excitons as well as a possible mechanism to further understand the charge-carrier dynamics in LPKs.