Giant enhancement of fluorescence resonance energy transfer based on nanoporous gold with small amount of residual silver.

Fluorescence resonance energy transfer (FRET) was found strongly enhanced by plasmon resonance. In this work, Nanoporous Gold with small amount of residual silver was used to form nanoporous gold/organic molecular layer compound with PSS and PAH. The ratio of its specific gold and silver content is achieved by controlling the time of its dealloying. Layered films of polyelectrolyte multilayers were assembled between the donor-acceptor pairs and NPG films to control distance. The maximum of FRET enhancement of 80-fold on the fluorescence intensity between the donor-acceptor pairs (CFP-YFP) is observed at a distance of ∼10.5 nm from the NPG film. This Nanoporous Gold with small amount of residual silver not only enhanced FRET 4-fold more than nanoporous gold of only gold content almost, but also effectively realized the regulation of FRET enhancement. The ability to precisely measure and regulate the enhancement of FRET enables the rational selection of plasmonic nanotransducer dimensions for the particular biosensing application.

Volume plasma grating by noncollinear interaction of femtosecond filament arrays.

Stable propagation of multifilament arrays in transparent bulk media with adjustable separation distances between adjacent child filaments has always been desired for advanced manufacturing. Here, we report on the generation of an ionization-induced volume plasma grating (VPG) by the interaction of two batches of noncollinearly propagating arrays of multiple filaments (AMF). The VPG can externally arrange the propagation of the pulses along regular plasma waveguides via spatial reconstruction of electrical fields, which is compared with the self-formation of randomly distributed multiple filamentation originated from noises. The separation distances of filaments in VPG are controllable by readily changing the crossing angle of the excitation beams. In addition, an innovative method to efficiently fabricate multidimensional grating structures in transparent bulk media through laser modification using VPG was demonstrated.

Synchronization, Desynchronization, and Intermediate Regime of Breathing Solitons and Soliton Molecules in a Laser Cavity.

We report on the experimental and numerical observations of synchronization and desynchronization of bound states of multiple breathing solitons (breathing soliton molecules) in an ultrafast fiber laser. In the desynchronization regime, although the breather molecules as wholes are not synchronized to the cavity, the individual breathers within a molecule are synchronized to each other with a delay (lag synchronization). An intermediate regime between the synchronization and desynchronization phases is also observed, featuring self-modulation of the synchronized state. This regime may also occur in other systems displaying synchronization. Breathing soliton molecules in a laser cavity open new avenues for the study of nonlinear synchronization dynamics.

Terahertz Time-of-Flight Ranging with Adaptive Clock Asynchronous Optical Sampling.

We propose and implement a terahertz time-of-flight ranging system based on adaptive clock asynchronous optical sampling, where the timing jitter is corrected in real time to recover the depth information in the acquired interferograms after compensating for laser instabilities using electronic signal processing. Consequently, the involved measurement uncertainties caused by the timing jitter during the terahertz sampling process and the noise intensity of the terahertz electric field have been reduced by the utilization of the adaptive clock. The achieved uncertainty range is about 2.5 µm at a 5 cm distance after averaging the acquisition time of 1876 ms 5000 times, showing a significant improvement compared with the asynchronous optical sampling using a constant clock. The implemented terahertz ranging system only uses free-running mode-locked lasers without any phase-locked electronics, and this favors simple and robust operations for subsequent applications that extend beyond the laboratory conditions.

Enhanced sequestration of CO2 from simulated electrolytic aluminum flue gas by modified red mud.

The aluminum industry is facing severe economic and environmental problems due to increasing carbon emissions and growing stockpiles of red mud (RM). RM is a strongly alkaline, high-emission solid waste from the alumina industry with potential for CO2 sequestration. However, the effectiveness of RM carbon sequestration is poor, and the mechanism behind it is not well understood. In this study, the effect of microwave and tube furnace activation of RM on CO2 sequestration in alumina was first investigated at different temperatures. The result showed that the CO2 sequestration capacity of unmodified RM (URM) was only 14.35 mg/g at ambient temperature and pressure, and the CO2 sequestration capacity could be increased to 52.89 mg/g after high-temperature activation and modification. Besides, high-temperature activation and modification will effectively improve the carbon sequestration capacity of RM. The carbonized RM was characterized by FT-IR, SEM, XRD, laser particle size, TG-DSC, and pH measurements. In addition, the mechanism of RM capturing CO2 was also proposed, which shows that CO2 was finally sequestered in the RM as CaCO3. The change in particle size distribution and the mineral phase in the RM indicated that high-temperature activation modification positively affects the application of RM to the sequestration of CO2. This study can provide a promising technology for the low-carbon and green development of the aluminum industry, as well as achieving the waste treatment and utilization objective.

High-speed photon-number-resolving detection via a GHz-gated SiPM.

Silicon photomultipliers (SiPMs) constitute a promising candidate for photon-number-resolving (PNR) detection via spatial multiplexing, which offer advantages like high integration and low cost. Up to date, there has been continuous endeavor in boosting the PNR performances, particularly on the resolved photon numbers and operation speed. Here, we demonstrate a GHz-gated SiPM in the Geiger mode, which allows to quench the photon-induced avalanche signal within 1 ns. Specifically, the capacitive response of the SiPM has been effectively suppressed by combining the low-pass filtering and self-differencing technique, which facilitates a high-fidelity extraction of the avalanche pulse with a reduced error rate. Consequently, high-speed PNR detection has been manifested in resolving up to 14 photons for laser pulses at a repetition rate of 40 MHz. The presented high-speed PNR detector may open up new possibilities to implement applications such as large-dynamic-range optical sensing, high-capacity optical communication, and multi-photon quantum optics.

Generation of broadband parabolic pulses based on a pre-chirper free, core-pumped nonlinear fiber amplifier for coherent anti-Stokes Raman imaging.

We report the generation of parabolic pulses with broadband spectrum from a core-pumped Yb-doped fiber amplifier seeded by a dispersion managed fiber oscillator. The net cavity dispersion of Yb-doped oscillator was continuously changed from 0.074 to -0.170 ps2, which enabled us to achieve dissipative soliton, stretched pulse and soliton mode-locking operations. Spectral evolution processes in the core-pumped nonlinear fiber amplifier seeded by various input solitons were investigated experimentally and theoretically. Our finding indicates that cavity dispersion of oscillator can be used to engineer the input pulse parameter for amplifier, thus forming a pre-chirper free fiber amplification structure. In the experiment, we obtained 410-mW parabolic pulses with spectral bandwidth up to 56 nm. In combination with a passively synchronized frequency-doubled Er-doped fiber laser, we have demonstrated coherent anti-Stokes Raman imaging. The compact dual-color fiber laser source may facilitate practical applications of nonlinear biomedical imaging beyond the laboratory environment.

Ultra-rapid dual-comb ranging with an extended non-ambiguity range.

In this Letter, we report a scheme that combines time-of-flight (ToF) ranging detection of multi-repetition-rate pulses with asymmetric dual-comb ranging (DCR) measurement. Notably, this combination extends the non-ambiguity range (NAR) of the DCR method without sacrificing its refresh rate and distance precision. With this scheme, we demonstrate absolute distance measurement of moving targets with an NAR of 1.5 km, which is 5× larger than that allowed solely by the DCR method for a given refresh rate at 500 kHz. The ranging precision in a single measurement of 2 µs reaches 10 µm at an effective distance of 571 m (down to 60 nm in 0.1 s). This combined scheme benefits remote sensing of high-speed objects.

Passive repetition-rate stabilization for a mode-locked fiber laser by electro-optic modulation.

We report a passive stabilization of the repetition rate for a mode-locked fiber laser by using an electro-optic modulator in a phase-biased nonlinear amplifying loop mirror. The underlying mechanism, in contrast to active feedback operations, lies in the cross-phase modulation between electrical and optical pulses within an electro-optic crystal. The resulting spectral shift can automatically compensate for the cavity-length drift via the group velocity dispersion. Consequently, the artificial actuator enables a capture range up to 2.3 mm, much longer than that achieved by index changes of the modulator. A robust and tight locking for the repetition rate is then realized with a standard deviation as low as 9 µHz with a 1-s sample time over 11 hours, corresponding to a fractional instability of 4.3 × 10-13. Furthermore, a dynamic optical sampling by repetition-rate tuning has been manifested with a fast refresh rate at 100 kHz and a broad scanning range over 305 ps. The demonstrated passive servo action may provide a simple yet effective way to stabilize the repetition rate with high precision, large bandwidth, and wide tunability.

High-precision passive stabilization of repetition rate for a mode-locked fiber laser based on optical pulse injection.

We have proposed and implemented a novel scheme to obtain high-precision repetition rate stabilization for a polarization-maintaining mode-locked fiber laser. The essential technique lies in the periodic injection of electronically modulated optical pulses into a nonlinear amplifying loop mirror within the laser resonator. Thanks to the nonlinear cross-phase modulation effect, the injected pulses referenced to an external clock serves as a stable and precise timing trigger for an effective intensity modulator. Consequently, synchronous mode-locking can be initiated to output ultrafast pulses with a passively stabilized repetition rate. The capture range of the locking system reaches to a record of 1 mm, which enables a long-term stable operation over 15 hours without the need of temperature stabilization and vibration isolation. Meanwhile, the achieved standard deviation is as low as 100 µHz with a 1-s sample time, corresponding to a fluctuation instability of 5.0×10-12. Additionally, the repetition rate stabilization performance based on the passive synchronization has been systematically investigated by varying the average power, central wavelength and pulse duration of the optical injection.

Surface plasmon enhanced THz emission with nanoporous gold supported CdTe.

Terahertz emission by ultrafast excitation of semiconductor/metal interfaces was found strongly enhanced by plasmon resonance. Here, a three-dimensional nanoporous gold (NPG) was used to form semiconductor/metal compound with cadmium telluride (CdTe). We investigated the specific impact of surface plasmon from randomly nanoporous structure in the ultrafast optoelectronic response for THz generation, and observed a THz amplitude enhancement around an order of magnitude from CdTe on NPG compared to that from CdTe on silicon. Moreover, the plasmon enhancement for THz emission from NPG is stronger than that from gold film, indicating that randomly nanoporous structure is also effective for plasmonic enhancement in THz band.

Realization of carrier envelope phase control in an erbium-doped all-fiber comb via an intracavity electrical polarization controller.

We present an erbium-doped all-fiber comb that is realized via intracavity piezoelectric mechanical responses by inserting an electrical polarization controller (EPC) for carrier envelope phase offset (fceo) control and sticking a piezoelectric transducer (PZT) for repetition rate (fr) stabilization. With only three components inside the oscillator, it facilitates an all-fiber comb system with high integration and robustness. Besides fceo control, smart, recoverable, and precise searching of mode-locked states can also be achieved by finely tuning the EPC driving voltages. The fceo signal can be tightly phase-locked due to the 20 kHz 3 dB bandwidth of the EPC device. Compared with the traditional pump feedback mode, the EPC approach exhibits a larger and flatter gain in the near-zero-dispersion zone of the fiber comb, corresponding to less EPC induced intracavity fluctuations. It is also a benefit for reducing cross regulation between fr and fceo in long-term stabilization of the comb.

High-order above-threshold dissociation of molecules.

Electrons bound to atoms or molecules can simultaneously absorb multiple photons via the above-threshold ionization featured with discrete peaks in the photoelectron spectrum on account of the quantized nature of the light energy. Analogously, the above-threshold dissociation of molecules has been proposed to address the multiple-photon energy deposition in the nuclei of molecules. In this case, nuclear energy spectra consisting of photon-energy spaced peaks exceeding the binding energy of the molecular bond are predicted. Although the observation of such phenomena is difficult, this scenario is nevertheless logical and is based on the fundamental laws. Here, we report conclusive experimental observation of high-order above-threshold dissociation of H2 in strong laser fields where the tunneling-ionized electron transfers the absorbed multiphoton energy, which is above the ionization threshold to the nuclei via the field-driven inelastic rescattering. Our results provide an unambiguous evidence that the electron and nuclei of a molecule as a whole absorb multiple photons, and thus above-threshold ionization and above-threshold dissociation must appear simultaneously, which is the cornerstone of the nowadays strong-field molecular physics.

Passively synchronized mode-locked fiber lasers for coherent anti-Stokes Raman imaging.

We have proposed and implemented a polarization-maintaining passively synchronized fiber laser system, which could deliver tunable dual-color picosecond pulses by including a frequency-doubling module and a spectral broadening module. Specifically, the output from the involved Er-doped fiber laser were used to generate second-harmonic pulses at 790 nm with a quadratic nonlinear crystal. In parallel, the amplified pulses from the synchronized Yb-doped fiber laser were launched into a 150-m single mode fiber, which resulted in not only substantial spectral bandwidth broadening from 0.1 to 20.1 nm, but also a significant Raman-induced signal around 1080 nm. Consequently, narrow spectra from 1018-1051 nm and 1070-1095 nm could be continuously tuned via a tunable bandpass filter, corresponding to Raman bonds from 2835-3143 cm-1 and 3312-3525 cm-1. Finally, the achieved tunable synchronized pulses enabled us to microscopically examine mouse ear samples based on coherent anti-Stokes Raman and second harmonic generation imaging. Therefore, our tunable passively-synchronized fiber laser system would be promising to provide a simple and compact laser source for subsequent coherent Raman microscopy.

Mid-infrared electro-optic dual-comb spectroscopy with feedforward frequency stepping.

In this Letter, we utilize an acoustic-optic frequency shifter in a feedforward manner for automatic interpolation of dual-comb spectroscopy, where frequency tuning can be achieved at 5.45 THz/s with the step size precisely locked to the line spacing (54.5 MHz) of a referenced optical comb without complicated electronics or control programs. Our dual-comb spectrometer involves two near-infrared electro-optic combs at 25 GHz line spacings, nonlinearly converted into the mid-infrared region, revealing fundamental absorption lines of methane gas at 54.5 MHz resolution within a spectral range from 88.04 to 89.04 THz. The method and the system may be useful in many applications, including gas sensing.

Fabrication of large scale uniform copper-island thin film for ultrasensitive surface enhanced Raman scattering.

Nanostructured metals with designable and controllable structures have received increasing attention in surface enhanced Raman scattering (SERS) due to the single molecular detection limit. Great challenges still remain in creating large scale substrates with high-density 'hotspots' to provide a uniform and stable enhancement of Raman signals. Here, we fabricated a copper island thin film over an 80 cm2 scale substrate with tunable particle sizes by combining sputtering with dealloying processes. The island size can be tailored from 150 nm to 370 nm by controlling parameters and etching conditions and possesses an optimized surface morphology structure. The detection limit of crystal violet (CV) molecules reached 0.1 pM. Meanwhile, the copper island thin film presents good homogeneity and stability. Our method is promising to repeatedly fabricate novel metal SERS substrates on a large scale with standard properties for sensing applications.

Fiber-based optical parametric oscillator with flexible repetition rates by rational harmonic pumping.

We demonstrated a fiber-based synchronously pumped optical parametric oscillator (SPOPO) with flexible repetition rates while retaining the cavity length. In contrast to conventional free-space SPOPO, the repetition rate of output signal pulses was solely determined by the repetition rate of the pump source in harmonic, fractional and rational operations. The relevant mechanism relies on synchronous pumping and intrinsic losses in our fiber resonator. The novel scheme enabled us to flexibly tune the repetition rate from 0.5 to 6.0 MHz without altering the resonator configuration. The resulting pulse properties were systematically analyzed at various operation conditions, and particularly showed that a wavelength tuning range of 157 nm was obtained. Such rational harmonic resonance implemented in our SPOPO provides not only a simple yet effective way to tune the repetition rate, but also a feasible approach to narrow down the spectral bandwidth. The presented SPOPO could be useful in nonlinear biomedical imaging by offering a convenient approach to optimize the pulse repetition rate for different biomedical samples with minimum photodamage.

Experimental study on buildup dynamics of a harmonic mode-locking soliton fiber laser.

In this paper, we experimentally investigate the onset dynamics of harmonic mode-locking (HML) in a short-cavity all-polarization-maintaining fiber laser using time-stretch spectroscopy. We observe a transient multi-pulse state evolving into a stable HML state. Moreover, a bunch of metastable short-lived mode-locking states are recorded before the laser entered the HML state. In these transient states, sudden changes including the formation and destruction of single broadband pulses are observed.

Observation of spectral mode splitting in a pump-enhanced ring cavity for mid-infrared generation.

We report on experimental and theoretical investigation of mode-splitting dynamics in a ring cavity under the perturbation of fractional Bragg reflection from a periodically-poled nonlinear crystal. Counterintuitively, pronounced mode splitting in the spectral domain could have been observed even with a tiny intensity reflection of 0.0003. The breaking of running-wave operation in the ring-cavity configuration resulted in comparable circulating fields in forward- and counter-propagation directions, which thus dramatically reduced the enhancing factor for the resonating field. In contrast, a linear cavity with intrinsically bidirectional operation was immune to the small intra-cavity reflection. Therefore, the linear-cavity layout could provide an expedient solution for a given internal reflection to obtain more stable and higher enhancement, which was confirmed by comparative studies of mid-infrared generation based on pump-enhanced difference frequency conversion. The underlying mechanism was further modeled by numerical simulations, which agreed well with experimental results. These findings could not only shed light on the understanding of the exotic feature of concatenated optical cavities, but also provide a useful guide to practical design of enhancement cavities for cavity-based frequency conversion with periodically-poled nonlinear crystals.

On the Q-switching bunch dynamics in the build-up of stretched-pulse mode-locking.

In this paper, we experimentally investigate a rich set of Q-switching bunches in the build-up of stretched-pulse mode-locking of an erbium-doped fiber laser. Interestingly, regular clustering of periodic Q-switched mode-locking states is observed in the self-starting process. Moreover, with time-stretch spectroscopy, we record periodic pulse-to-pulse spectral evolution occurring in these turbulent and rapidly-evolving pre-mode-locking states.