Abstract
Transition metal dichalcogenides have been widely utilized as nonlinear optical materials for laser pulse generation applications. Herein, we study the nonlinear optical properties of a VS2-based optical device and its application as a new saturable absorber (SA) for high-power pulse generation. Few-layer VS2 nanosheets are deposited on the tapered region of a microfiber to form an SA device, which shows a modulation depth of 40.52%. After incorporating the microfiber-VS2 SA into an Er-doped fiber laser cavity, passively Q-switched pulse trains could be obtained with repetition rates varying from 95 to 233 kHz. Under the pump power of 890 mW, the largest output power and shortest pulse duration are measured to be 43 mW and 854 ns, respectively. The high signal-to-noise ratio of 60 dB confirms the excellent stability of the Q-switching state. To the best of our knolowdge, this is the first illustration of using VS2 as an SA. Our experimental results demonstrate that VS2 nanomaterials have a large potential for nonlinear optics applications.
1 Introduction
Nonlinear optical materials, as fundamental components of electronic and optoelectronic devices, play a key role in the field of advanced photonics [1], [2], [3], [4], [5], [6]. In recent decades, widespread attention has been paid to investigate these promising materials, which has become a research hotspot [7], [8], [9], [10]. Some low-dimensional nanomaterials with outstanding attributes of fast response, low cost, wideband linear optical absorption, high optical nonlinearity and simplicity of integrating into an optical system have been proved to be effective nonlinear optical materials [11], [12], [13], [14], [15], [16]. Particularly, two-dimensional (2D) materials are developed for wide applications in the nonlinear optical field because of their attractive photonic characteristics, including ultrafast carrier dynamics, strong light-matter interaction and large modulation depth. Consequently, the 2D materials provide a good platform for potential optical applications of, for example, optical modulation, optical limiting and photodetectors [17], [18].
As we all know, the pulse lasers have various applications such as basic physics, precision material processing and health care. Passively mode-locking and Q-switching techniques are the two main ways to generate pulses, whose prospective applications are on the rise [19], [20], [21]. Currently, graphene [22], topological insulators (TIs) [23], metal–organic frameworks [24], [25], perovskite [26], MXene [27], group-VA mono-elemental materials [28], [29], [30], transition metal dichalcogenides (TMDCs) [31], [32], black phosphorus [33], [34], [35] and IIIA/IVA monochalcogenides [36] have been extensively investigated and confirmed as great alternatives to saturable absorbers (SAs) in pulsed laser systems for ultrashort pulse generation. In the past few years, extensive efforts have been made to use TMDCs as SAs to induce Q-switching and mode locking over a wide wavelength range from visible to near infrared, which exhibits tunable bandgap, low optical attenuation and nonlinear optical effect generation [37], [38]. The general term TMDC is used to refer to the combination of chalcogen atoms (S, Se and Te) and transition metals (groups IVB to VIII, IB, and IIB). Actually, the group VIB TMDCs (MoS2 and WS2) have been used for pulse generation thoroughly [39], [40]. Furthermore, some other TMDCs with a small bandgap, including ReS2 and HfS2, have also been used as SAs [41], [42]. However, the VB TMDC-based ultrafast photonics devices remain at the initial stage of development [43]. VS2, as a representative conducting VB TMDC, consists of a metal vanadium sandwiched between the two sulfide layers as S-V-S, exhibiting metallic behavior with negligible bandgap [44]. Due to a wealth of intriguing properties of magnetism, charge density waves, and superconductivity, VS2 has particular advantages for multifunctional applications in the field of supercapacitor, nanoelectronics, energy storage and hydrogen evolution [45], [46]. To the best of our knowledge, there has been no research devoted to the nonlinear optical property of VS2.
In this study, we have prepared a microfiber-VS2 device and used it as a new SA for high-power nanosecond Q-switched pulse generation. VS2 nanosheet dispersion is fabricated via the liquid exfoliation method using N-methylpyrrolidone (NMP) as a solvent. Then, the VS2 nanosheets are deposited on the tapered region of a microfiber to form an SA device, which shows the modulation depth of 40.52%. Based on VS2 saturable absorption, passively Q-switched pulses are generated in the EDF laser. The maximum output power/minimum pulse duration is 43 mW/854 ns under the pump power of 890 mW. The signal-to-noise ratio (SNR) up to 60 dB confirms good stability of a Q-switched fiber laser. These experimental results indicate that VS2 can be used as a remarkable SA material for high-power pulse generation.
2 Experiments
2.1 Preparation of a microfiber-VS2 SA
Top to down methods are the common techniques to make layered structure materials from bulk to few layers. Depending on the fabrication conditions, the nanometer sizes can be tunable. Figure 1A depicts the VS2 lattice structure. The interval between two layers is 5.76 Å. Liquid phase exfoliation may be an ideal process to fabricate VS2 nanosheets with the advantages of easy preparation and high quality. The detailed fabrication process was as follows. First, the bulk VS2 crystal was ground into powder. The second step was the sonification procedure. The 10 mg VS2 powder and 20 ml NMP solvent were mixed. Afterward, the mixed solution underwent ultrasonication for 8 h. The NMP has been demonstrated to be a good solvent for exfoliating 2D materials, whose surface energy matches well with VS2 nanosheets [47]. So we do not utilize surfactant as the assisted medium. During this process, the VS2 nanosheets with different thicknesses were chopped with the aid of sonication energy and temporarily stabilized by physically interacting with the NMP solvent. Few-layered VS2 nanosheets were obtained via the next centrifugation process. The VS2 nanosheet dispersion is shown in Figure 1B. Raman spectra are displayed in Figure 1C. The E1g and A1g active modes locate at 281 and 373 cm−1, corresponding to in-plane and out-of-plane vibrations of VS2. Figure 2 shows the atomic force microscopy (AFM) image of VS2 nanosheets. The cross-section height profile along four dotted lines indicates the thickness of VS2 nanosheets ranging from 17 to 20 nm. The indirect evanescent field coupling approach is developed to construct the VS2-based SA device, which can realize stabilizing and strong light-matter interaction between light and VS2 nanosheets. The microfiber-VS2 SA is formed by depositing VS2 nanosheets onto the side surface of a microfiber when the laser passes through the microfiber. The waist diameter of the taper is set to be 12 μm and the length of it is 2 mm. The taper waist of 12 μm leads to a strong evanescent-material interaction. The interaction length of 2 mm enables the VS2 nanosheets take full advantages of the modulation ability.

The characters of VS2.
(A) The lattice structure of VS2; (B) the photograph of VS2 nanosheet dispersion; (C) Raman spectra of VS2.

AFM image and the corresponding height profile.
2.2 Laser configuration
The laser structure is schematically shown in Figure 3. The pump source is a laser diode with output power adjusting from 0 to 900 mW. A 980/1550 wavelength division multiplexer connects the pump source and resonant cavity. The length of the gain fiber (ER110-4/125, Thorlabs, Inc., Newton, NJ, USA) is selected to be 35 cm. The fiber polarization independent isolator is set to ensure the laser unidirectional transmission but not filter the polarization direction. The SA is a piece of microfiber coated with VS2 nanosheets. The waist region is tightly straightened and fixed on the quartz flake. The output port is a 50/50 optical coupler and the pigtail fiber is about 50 cm SMF-28e fiber. The pigtail fiber of all optical elements is SMF-28e fiber and the total cavity length is about 3.9 m. The measuring instruments include the following: a 1 GHz bandwidth and 10GSa/s digital oscilloscope (Rohde & Schwarz RTO2014, Munich, Germany), a 13.6 GHz radio frequency (RF) spectrum analyzer (Rohde & Schwarz FSW13, Munich, Germany), an optical spectrum analyzer (YOKOGAWA AQ6370D, Tokyo, Japan), and a fiber optical power meter (VIAVI OLP-85, JDSU, Breinigsville, PA, USA).

Schematic illustration of the Q-switched EDF laser based on the microfiber-VS2 SA.
3 Results and discussion
3.1 The nonlinear optical absorption of SA
The linear transmittance of the microfiber-VS2 SA is measured from 1500 to 1600 nm. As depicted in Figure 4A, the transmittance is 46.4% at 1550 nm. The balanced twin detector measurement is used to judge the nonlinear optical response characteristics of the microfiber-VS2 device. A nonlinear polarization rotation mode-locked EDF laser acts as the optical source, which operates at 1556 nm with a repetition rate of 42 MHz and a pulse duration of 600 fs. Figure 4B shows the dependence of transmittance on the incident laser peak power density. According to the two-level saturable absorption model, the nonlinear optical absorption of the proposed SA device is fitted by the following equation:

The optical characteristics of microfiber-VS2 SA.
(A) The linear transmittance of the microfiber-VS2 SA; (B) the nonlinear optical absorption curve of the microfiber-VS2 SA.
where the saturable intensity (Isat), nonsaturable loss (αns) and modulation depth (∆T) are calculated to be 18.06 MW/cm2, 15.07%, and 40.52%, respectively.
3.2 Q-switched operation
In this experiment, Q-switching operation can be obtained under the pump power of 150–890 mW. Figure 5A shows the Q-switched pulse train evolution depending on different pump powers. With increasing pump power, the pulse period and pulse width decrease gradually. Fixing the pump power at 890 mW, we measured the shortest pulse duration to be 854 ns, which is shown in Figure 5B. The related optical spectrum characteristics are depicted in Figure 5C. It can be seen that the spectral shape with the central wavelength of 1531 nm remains almost unchanged. While the 3-dB bandwidth widens to 4 nm slowly with the pump power increasing to 890 mW. Setting the resolution bandwidth to be 200 Hz, we measured the RF spectrum in the span of 510 kHz at the pump power of 890 mW. As demonstrated in Figure 5D, the repetition rate locates at 233 kHz with the SNR of 60 dB, confirming the good stability of this Q-switched fiber laser. Figure 5E depicts the typical features of the Q-switched fiber laser. The repetition rate is expanded from 95 to 233 kHz and the pulse width is lowered from 4.27 μs to 854 ns as the pump power is increased from 150 to 890 mW. As shown in Figure 5F, in the pump range of 150–890 mW, the average output power increases from 3.58 to 43 mW almost linearly. The single pulse energy enlarges from 36.9 to 184.6 nJ monotonically. Under the pump power of 850 mW, we keep this Q-switched fiber laser working 2 h a day for 10 consecutive days. We note that the pulse trains remain stable with no appearance of pulse splitting, indicating that the long-term stability of working is good. It is widely accepted that the mode-locked pulse characteristics are determined by the interaction of dispersion and nonlinear effects. In this work, the dispersion and nonlinearity have not reached equilibrium. Besides, the 50/50 optical coupler is used. Therefore, the intra-cavity power is relatively low. Thus, the passive mode-locking phenomenon does not appear.

Experimental results.
(A) The Q-switched pulse sequence at different pump powers; (B) single pulse duration at the pump power of 890 mW; (C) the optical spectrum; (D) the RF spectrum; (E) relationship of pump power and repetition rate (pulse width); (F) relationship of pump power and output power (pulse energy).
Table 1 demonstrates the output performances of passively Q-switched EDF lasers to compare the nonlinear optical response of VS2-based SA with the same kind of SAs using other 2D materials. The modulation depth of 40.52% is much larger than that of other SAs, which is originated from the evanescent field coupling mechanism. This scheme can increase the interaction length between light and VS2 materials; therefore, the nonlinearity of the VS2-based SA device would be enhanced. So the modulation of light is stronger. For the pulse duration comparison, the pulse duration of listed Q-switched fiber lasers is mostly in the μs time scale, while ns-level Q-switched pulses are obtained in our experiment. The repetition rate range of 95–233 kHz and the maximum pulse energy of 184.6 nJ in the current work are competitive to that of previous reports. Notably, the maximum output power of 43 mW is much higher than that of passively Q-switched EDF lasers with other 2D materials. Overall, our results are superior to other works in terms of modulation depth, pulse duration, pulse energy and average output power. The saturable absorption process of VS2 can be explained by the Pauli blocking principle. When weak-intensity incident light illuminates the VS2 material, the light can excite electrons from the valence band into the conduction band. These photon-generated hot carriers cool down rapidly and form a hot Fermi-Dirac distribution. Thus the newly formed electron-hole pairs would suppress the inter-band photon transition. Next, the electron-hole pair recombination dominates until the distribution of electrons and holes returns to equilibrium. When the light intensity is strong enough, the photon-generated carriers rise immediately and occupy the energy states nearby the edge of the conduction and valence band completely. Because of the Pauli blocking principle, the photons pass through without loss.
Comparison of the performances of Q-switched EDF lasers based on different 2D SAs.
SA | ΔT (%) | Repetition rate, kHz | Pulse width, μs | Output power, mW | Pulse energy, nJ | Reference |
---|---|---|---|---|---|---|
Graphene | 45 | 3.3–69.5 | 3.7 | 1.1 | 16.7 | [48] |
Black phosphorus | 0.47 | 5.73–31.07 | 3.59 | 4.2 | 142.6 | [49] |
CH3NH3PbI3 | – | 15.2–36.4 | 0.919 | 28 | 770 | [50] |
SnS | 36.4 | 36.36–65.19 | – | 1.1 | – | [51] |
ReS2 | 0.12 | 12.6–19 | 5.496 | 1.2 | 62.8 | [52] |
TiS2 | 8.3 | 25.2–50.7 | 4 | 0.48 | 9.46 | [53] |
WS2 | 2.9 | 90–125 | – | 5.7 | 46.3 | [54] |
TiSe2 | 25.92 | 70–154 | 1.126 | 11.54 | 74.9 | [55] |
HfSe2 | 6.65 | 12.97–45 | 4.5 | 7.5 | 167 | [56] |
MoSe2 | 21.7 | 47.5–105.7 | 1.09 | 23.2 | 224 | [57] |
PtSe2 | 4.9 | 20.5–79.2 | 0.92 | 11.34 | 143.2 | [58] |
VS2 | 40.52 | 95–233 | 0.854 | 43 | 184.6 | This work |
4 Conclusion
In summary, we introduced the new 2D nanomaterial VS2 as a SA into the EDF laser for the first time. VS2 nanosheets coated onto the microfiber form the SA device simply with the modulation depth of 40.52%. The repetition rate can be adjusted in the range of 95–233 kHz. The SNR of 60 dB confirms the stability of the Q-switched fiber laser. The maximum output power and shortest pulse duration are 43 mW and 854 ns at the pumper power of 890 mW. This work illustrates that VS2 is a promising candidate of SA for the pulsed fiber laser with excellent output performance.
Acknowledgments
This work was supported by the National Natural Science Foundation of China (NSFC) (Nos. 61705183, 11875044, Funder Id: http://dx.doi.org/10.13039/501100001809); the Nature Science Foundation of Shaanxi Province, China (Nos. 2019JQ-446, 2019JM-131); Young Talent fund of University Association for Science and Technology in Shaanxi, China (No. 20190113); and Science Research Foundation of the Education Department of Shaanxi Province, China (No. 19JK0811).
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© 2020 Lu Li, Wenjun Liu et al., published by De Gruyter, Berlin/Boston
This work is licensed under the Creative Commons Attribution 4.0 Public License.
Articles in the same Issue
- Reviews
- All-optical modulation with 2D layered materials: status and prospects
- Two-dimensional metal carbides and nitrides (MXenes): preparation, property, and applications in cancer therapy
- Novel two-dimensional monoelemental and ternary materials: growth, physics and application
- Solution-processed two-dimensional materials for ultrafast fiber lasers (invited)
- Recent advances on hybrid integration of 2D materials on integrated optics platforms
- Recent progress of pulsed fiber lasers based on transition-metal dichalcogenides and black phosphorus saturable absorbers
- Two-dimensional MXene-based materials for photothermal therapy
- Advances in inorganic and hybrid perovskites for miniaturized lasers
- Visible-wavelength pulsed lasers with low-dimensional saturable absorbers
- Hybrid silicon photonic devices with two-dimensional materials
- Recent advances in mode-locked fiber lasers based on two-dimensional materials
- Research Articles
- Ternary chalcogenide Ta2NiS5 nanosheets for broadband pulse generation in ultrafast fiber lasers
- All-optical dynamic tuning of local excitonic emission of monolayer MoS2 by integration with Ge2Sb2Te5
- Dual-wavelength dissipative solitons in an anomalous-dispersion-cavity fiber laser
- Physical vapor deposition of large-scale PbSe films and its applications in pulsed fiber lasers
- Double-layer graphene on photonic crystal waveguide electro-absorption modulator with 12 GHz bandwidth
- Resonance-enhanced all-optical modulation of WSe2-based micro-resonator
- Black phosphorus-Au nanocomposite-based fluorescence immunochromatographic sensor for high-sensitive detection of zearalenone in cereals
- Lanthanide Nd ion-doped two-dimensional In2Se3 nanosheets with near-infrared luminescence property
- Broadband spatial self-phase modulation and ultrafast response of MXene Ti3C2Tx (T=O, OH or F)
- PEGylated-folic acid–modified black phosphorus quantum dots as near-infrared agents for dual-modality imaging-guided selective cancer cell destruction
- Dynamic polarization attractors of dissipative solitons from carbon nanotube mode-locked Er-doped laser
- Environmentally stable black phosphorus saturable absorber for ultrafast laser
- MXene saturable absorber enabled hybrid mode-locking technology: a new routine of advancing femtosecond fiber lasers performance
- Solar-blind deep-ultraviolet photodetectors based on solution-synthesized quasi-2D Te nanosheets
- Enhanced photoresponse of highly air-stable palladium diselenide by thickness engineering
- MoS2-based Charge-trapping synaptic device with electrical and optical modulated conductance
- Multifunctional black phosphorus/MoS2 van der Waals heterojunction
- MXene Ti3C2Tx saturable absorber for passively Q-switched mid-infrared laser operation of femtosecond-laser–inscribed Er:Y2O3 ceramic channel waveguide
- MXene: two dimensional inorganic compounds, for generation of bound state soliton pulses in nonlinear optical system
- Layered iron pyrite for ultrafast photonics application
- 2D molybdenum carbide (Mo2C)/fluorine mica (FM) saturable absorber for passively mode-locked erbium-doped all-fiber laser
- Ultrasensitive graphene position-sensitive detector induced by synergistic effects of charge injection and interfacial gating
- Two-dimensional Au & Ag hybrid plasmonic nanoparticle network: broadband nonlinear optical response and applications for pulsed laser generation
- The SnSSe SA with high modulation depth for passively Q-switched fiber laser
- Palladium selenide as a broadband saturable absorber for ultra-fast photonics
- VS2 as saturable absorber for Q-switched pulse generation
- Highly stable MXene (V2CTx)-based harmonic pulse generation
- Simultaneously enhanced linear and nonlinear photon generations from WS2 by using dielectric circular Bragg resonators
- 2D tellurene/black phosphorus heterojunctions based broadband nonlinear saturable absorber
Articles in the same Issue
- Reviews
- All-optical modulation with 2D layered materials: status and prospects
- Two-dimensional metal carbides and nitrides (MXenes): preparation, property, and applications in cancer therapy
- Novel two-dimensional monoelemental and ternary materials: growth, physics and application
- Solution-processed two-dimensional materials for ultrafast fiber lasers (invited)
- Recent advances on hybrid integration of 2D materials on integrated optics platforms
- Recent progress of pulsed fiber lasers based on transition-metal dichalcogenides and black phosphorus saturable absorbers
- Two-dimensional MXene-based materials for photothermal therapy
- Advances in inorganic and hybrid perovskites for miniaturized lasers
- Visible-wavelength pulsed lasers with low-dimensional saturable absorbers
- Hybrid silicon photonic devices with two-dimensional materials
- Recent advances in mode-locked fiber lasers based on two-dimensional materials
- Research Articles
- Ternary chalcogenide Ta2NiS5 nanosheets for broadband pulse generation in ultrafast fiber lasers
- All-optical dynamic tuning of local excitonic emission of monolayer MoS2 by integration with Ge2Sb2Te5
- Dual-wavelength dissipative solitons in an anomalous-dispersion-cavity fiber laser
- Physical vapor deposition of large-scale PbSe films and its applications in pulsed fiber lasers
- Double-layer graphene on photonic crystal waveguide electro-absorption modulator with 12 GHz bandwidth
- Resonance-enhanced all-optical modulation of WSe2-based micro-resonator
- Black phosphorus-Au nanocomposite-based fluorescence immunochromatographic sensor for high-sensitive detection of zearalenone in cereals
- Lanthanide Nd ion-doped two-dimensional In2Se3 nanosheets with near-infrared luminescence property
- Broadband spatial self-phase modulation and ultrafast response of MXene Ti3C2Tx (T=O, OH or F)
- PEGylated-folic acid–modified black phosphorus quantum dots as near-infrared agents for dual-modality imaging-guided selective cancer cell destruction
- Dynamic polarization attractors of dissipative solitons from carbon nanotube mode-locked Er-doped laser
- Environmentally stable black phosphorus saturable absorber for ultrafast laser
- MXene saturable absorber enabled hybrid mode-locking technology: a new routine of advancing femtosecond fiber lasers performance
- Solar-blind deep-ultraviolet photodetectors based on solution-synthesized quasi-2D Te nanosheets
- Enhanced photoresponse of highly air-stable palladium diselenide by thickness engineering
- MoS2-based Charge-trapping synaptic device with electrical and optical modulated conductance
- Multifunctional black phosphorus/MoS2 van der Waals heterojunction
- MXene Ti3C2Tx saturable absorber for passively Q-switched mid-infrared laser operation of femtosecond-laser–inscribed Er:Y2O3 ceramic channel waveguide
- MXene: two dimensional inorganic compounds, for generation of bound state soliton pulses in nonlinear optical system
- Layered iron pyrite for ultrafast photonics application
- 2D molybdenum carbide (Mo2C)/fluorine mica (FM) saturable absorber for passively mode-locked erbium-doped all-fiber laser
- Ultrasensitive graphene position-sensitive detector induced by synergistic effects of charge injection and interfacial gating
- Two-dimensional Au & Ag hybrid plasmonic nanoparticle network: broadband nonlinear optical response and applications for pulsed laser generation
- The SnSSe SA with high modulation depth for passively Q-switched fiber laser
- Palladium selenide as a broadband saturable absorber for ultra-fast photonics
- VS2 as saturable absorber for Q-switched pulse generation
- Highly stable MXene (V2CTx)-based harmonic pulse generation
- Simultaneously enhanced linear and nonlinear photon generations from WS2 by using dielectric circular Bragg resonators
- 2D tellurene/black phosphorus heterojunctions based broadband nonlinear saturable absorber