2D transition metal carbides, nitrides, and carbonitides called MXenes have attracted much attention due to their outstanding properties. However, MXene's potential in laser technology is not explored. It is demonstrated here that Ti CN, one of MXene compounds, can serve as an excellent mode-locker that can produce femtosecond laser pulses from fiber cavities. Stable laser pulses with a duration as short as 660 fs are readily obtained at a repetition rate of 15.4 MHz and a wavelength of 1557 nm. Density functional theory calculations show that Ti CN is metallic, in contrast to other 2D saturable absorber materials reported so far to be operative for mode-locking. 2D structural and electronic characteristics are well conserved in their stacked form, possibly due to the unique interlayer coupling formed by MXene surface termination groups. Noticeably, the calculations suggest a promise of MXenes in broadband saturable absorber applications due to metallic characteristics, which agrees well with the experiments of passively Q-switched lasers using Ti CN at wavelengths of 1558 and 1875 nm. This study provides a valuable strategy and intuition for the development of nanomaterial-based saturable absorbers opening new avenues toward advanced photonic devices based on MXenes.

Tungsten ditelluride (WTe2) is a layered material that exhibits excellent magnetoresistance and thermoelectric behaviors, which are deeply related with its distorted orthorhombic phase that may critically affect the lattice dynamics of this material. Here, we report comprehensive characterization of Raman spectra of WTe2 from bulk to monolayer using experimental and computational methods. We find that mono and bi-layer WTe2 are easily identified by Raman spectroscopy since two or one Raman modes that are observed in higher-layer WTe2 are greatly suppressed below the noise level in the mono- and bi-layer WTe2, respectively. In addition, the frequency of in-plane A1(7) mode of WTe2 remains almost constant as the layer number decreases, while all the other Raman modes consistently blueshift, which is completely different from the vibrational behavior of hexagonal metal dichalcogenides. First-principles calculation validates experimental results and reveals that anomalous lattice vibrations in WTe2 are attributed to the formation of tungsten chains that make WTe2 structurally one-dimensional.

Mono‐ and few‐layer transition metal dichalcogenides (TMDCs) have been widely used as saturable absorbers for ultrashort laser pulse generation, but their preparation is complicated and requires much expertise. The possible use of bulk‐structured TMDCs as saturable absorbers is therefore a very intriguing and technically important issue in laser technology. Here, for the first time, it is demonstrated that defective, bulk‐structured WTe2 microflakes can serve as a base saturable absorption material for fast mode‐lockers that can produce femtosecond pulses from fiber laser cavities. They have a modulation depth of 2.85%, from which stable laser pulses with a duration of 770 fs are readily obtained at a repetition rate of 13.98 MHz and a wavelength of 1556.2 nm, which is comparable to the performance achieved using mono‐ and few‐layer TMDCs. Density functional theory calculations show that the oxidative and defective surfaces of WTe2 microflakes do not degrade their saturable absorption performance in the near‐infrared range, allowing for a broad range of operative bandwidth. This study suggests that saturable absorption is an intrinsic property of TMDCs without relying on their structural dimensionality, providing a new direction for the development of TMDC‐based saturable absorbers.

Monolayer MoS2 (1L-MoS2) has photoluminescence (PL) properties that can greatly vary via transition between neutral and charged exciton PLs depending on carrier density. Here, for the first time, we present a chemical doping method for reversible transition between neutral and charged excitons of 1L-MoS2 using chlorine-hydrogen-based plasma functionalization. The PL of 1L-MoS2 is drastically increased by p-type chlorine plasma doping in which its intensity is easily tuned by controlling the plasma treatment duration. We find that despite their strong adhesion, a post hydrogen plasma treatment can very effectively dedope chlorine adatoms in a controllable way while maintaining robust structural integrity, which enables well-defined reversible PL control of 1L-MoS2. After exhaustive chlorine dedoping, the hydrogen plasma process induces n-type doping of 1L-MoS2, degrading the PL further, which can also be recovered by subsequent chlorine plasma treatment, extending the range of tunable PL into a bidirectional regime. This cyclically-tunable carrier doping method can be usefully employed in fabricating highly-tunable n- and p-type domains in monolayer transition-metal dichalcogenides suitable for two-dimensional electro-optic modulators, on-chip lasers, and spin- and valley-polarized light-emitting diodes.

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