Valleytronics in bulk MoS2 with a topologic optical field.

The valley degree of freedom1-4 of electrons in materials promises routes towards energy-efficient information storage with enticing prospects for quantum information processing5-7. Current challenges in utilizing valley polarization are symmetry conditions that require monolayer structures8,9 or specific material engineering10-13, non-resonant optical control to avoid energy dissipation and the ability to switch valley polarization at optical speed. We demonstrate all-optical and non-resonant control over valley polarization using bulk MoS2, a centrosymmetric material without Berry curvature at the valleys. Our universal method utilizes spin angular momentum-shaped trefoil optical control pulses14,15 to switch the material's electronic topology and induce valley polarization by transiently breaking time and space inversion symmetry16 through a simple phase rotation. We confirm valley polarization through the transient generation of the second harmonic of a non-collinear optical probe pulse, depending on the trefoil phase rotation. The investigation shows that direct optical control over the valley degree of freedom is not limited to monolayer structures. Indeed, such control is possible for systems with an arbitrary number of layers and for bulk materials. Non-resonant valley control is universal and, at optical speeds, unlocks the possibility of engineering efficient multimaterial valleytronic devices operating on quantum coherent timescales.

Three-photon head-mounted microscope for imaging deep cortical layers in freely moving rats.

We designed a head-mounted three-photon microscope for imaging deep cortical layer neuronal activity in a freely moving rat. Delivery of high-energy excitation pulses at 1,320 nm required both a hollow-core fiber whose transmission properties did not change with fiber movement and dispersion compensation. These developments enabled imaging at >1.1 mm below the cortical surface and stable imaging of layer 5 neuronal activity for >1 h in freely moving rats performing a range of behaviors.

Optofluidic Photonic Crystal Fiber Microreactors for In Situ Studies of Carbon Nanodot-Driven Photoreduction.

Performing quantitative in situ spectroscopic analysis on minuscule sample volumes is a common difficulty in photochemistry. To address this challenge, we use a hollow-core photonic crystal fiber (HC-PCF) that guides light at the center of a microscale liquid channel and acts as an optofluidic microreactor with a reaction volume of less than 35 nL. The system was used to demonstrate in situ optical detection of photoreduction processes that are key components of many photocatalytic reaction schemes. The photoreduction of viologens (XV2+) to the radical XV•+ in a homogeneous mixture with carbon nanodot (CND) light absorbers is studied for a range of different carbon dots and viologens. Time-resolved absorption spectra, measured over several UV irradiation cycles, are interpreted with a quantitative kinetic model to determine photoreduction and photobleaching rate constants. The powerful combination of time-resolved, low-volume absorption spectroscopy and kinetic modeling highlights the potential of optofluidic microreactors as a highly sensitive, quantitative, and rapid screening platform for novel photocatalysts and flow chemistry in general.

Efficient self-compression of ultrashort near-UV pulses in air-filled hollow-core photonic crystal fibers.

We report generation of ultrashort near-UV pulses by soliton self-compression in kagomé-style hollow-core photonic crystal fibers filled with ambient air. Pump pulses with the energy of 2.6 µJ and duration of 54 fs at 400 nm were compressed temporally by a factor of 5, to a duration of ∼11 fs. The experimental results are supported by numerical simulations, showing that both Raman and Kerr effects play a role in the compression dynamics. The convenience of using ambient air and the absence of glass windows that would distort the compressed pulses makes the setup highly attractive as the basis of an efficient table-top UV pulse compressor.

Scaling rules for high quality soliton self-compression in hollow-core fibers.

Soliton dynamics can be used to temporally compress laser pulses to few fs durations in many different spectral regions. Here we study analytically, numerically and experimentally the scaling of soliton dynamics in noble gas-filled hollow-core fibers. We identify an optimal parameter region, taking account of higher-order dispersion, photoionization, self-focusing, and modulational instability. Although for single-shots the effects of photoionization can be reduced by using lighter noble gases, they become increasingly important as the repetition rate rises. For the same optical nonlinearity, the higher pressure and longer diffusion times of the lighter gases can considerably enhance the long-term effects of ionization, as a result of pulse-by-pulse buildup of refractive index changes. To illustrate the counter-intuitive nature of these predictions, we compressed 250 fs pulses at 1030 nm in an 80-cm-long hollow-core photonic crystal fiber (core radius 15 µm) to ∼5 fs duration in argon and neon, and found that, although neon performed better at a repetition rate of 1 MHz, stable compression in argon was still possible up to 10 MHz.

Doppler optical frequency domain reflectometry for remote fiber sensing: erratum.

This erratum corrects a typographical error in Eq. (10) of our paper [Opt. Express29, 14615 (2021)10.1364/OE.421842].

Reconfigurable millimeter-range optical binding of dielectric microparticles in hollow-core photonic crystal fiber.

Optical binding of microparticles offers a versatile playground for investigating the optomechanics of levitated multi-particle systems. We report millimeter-range optical binding of polystyrene microparticles in hollow-core photonic crystal fiber. The first particle scatters the incident LP01 mode into several LP0n modes, creating a beat pattern that exerts a position-dependent force on the second particle. Particle binding results from the interplay of the forces created by counterpropagating beams. A femtosecond trapping laser is used so that group velocity walk-off eliminates disturbance caused by higher order modes accidentally excited at the fiber input. The inter-particle distance can be optically switched over 2 orders of magnitude (from 42 µm to 3 mm), and the bound particle pairs can be translated along the fiber by unbalancing the powers in the counterpropagating trapping beams. The frequency response of a bound particle pair is investigated at low gas pressure by driving with an intensity-modulated control beam. The system offers new degrees of freedom for manipulating the dynamics and configurations of optically levitated microparticle arrays.

Deep-UV-enhanced supercontinuum generated in a tapered gas-filled photonic crystal fiber.

We present the use of a linearly down-tapered gas-filled hollow-core photonic crystal fiber in a single stage, pumped with pulses from a compact infrared (IR) laser source, to generate a supercontinuum (SC) carrying significant spectral power in the deep ultraviolet (UV) [200-300 nm]. The generated SC extends from the near IR down to ∼213nm with 0.58 mW/nm and down to ∼220nm with 0.83 mW/nm in the deep UV.

Cross-phase modulational instability of circularly polarized helical Bloch modes carrying optical vortices in a chiral three-core photonic crystal fiber.

We report the first, to the best of our knowledge, observation of cross-phase modulational instability (XPMI) of circularly polarized helical Bloch modes carrying optical vortices in a twisted photonic crystal fiber with a three-fold symmetric core, formed by spinning the fiber preform during the draw. When the fiber is pumped by a superposition of left-circular polarization (LCP) and right-circular polarization (RCP) modes, a pair of orthogonal circularly polarized sidebands of opposite topological charge is generated. When, on the other hand, a pure LCP (or RCP) mode is launched, the XPMI gain is zero, and no sidebands are seen. This observation has not been seen before in any system and is unique to chiral structures with N-fold rotational symmetry. The polarization state and topological charge of the generated sidebands are measured. By decomposing the helical Bloch modes into their azimuthal harmonics, we are able to deduce the selection rules for the appearance of modulational instability sidebands. We showed that the four waves in the nonlinear mixing process must exhibit the same set of azimuthal harmonic orders.

Covariance spectroscopy of molecular gases using fs pulse bursts created by modulational instability in gas-filled hollow-core fiber.

We present a technique that uses noisy broadband pulse bursts generated by modulational instability to probe nonlinear processes, including infrared-inactive Raman transitions, in molecular gases. These processes imprint correlations between different regions of the noisy spectrum, which can be detected by acquiring single shot spectra and calculating the Pearson correlation coefficient between the different frequency components. Numerical simulations verify the experimental measurements and are used to further understand the system and discuss methods to improve the signal strength and the spectral resolution of the technique.

Modulational-instability-free pulse compression in anti-resonant hollow-core photonic crystal fiber.

Gas-filled hollow-core photonic crystal fiber (PCF) is used for efficient nonlinear temporal compression of femtosecond laser pulses, two main schemes being direct soliton-effect self-compression and spectral broadening followed by phase compensation. To obtain stable compressed pulses, it is crucial to avoid decoherence through modulational instability (MI) during spectral broadening. Here, we show that changes in dispersion due to spectral anti-crossings between the fundamental-core mode and core wall resonances in anti-resonant-guiding hollow-core PCF can strongly alter the MI gain spectrum, enabling MI-free pulse compression for optimized fiber designs. The results are important, since MI cannot always be suppressed by pumping in the normal dispersion regime.

Generation of 1.5 cycle pulses at 780 nm at oscillator repetition rates with stable carrier-envelope phase.

We demonstrate a spectral broadening and compression setup for carrier-envelope phase (CEP) stable sub-10-fs Ti:sapphire oscillator pulses resulting in 3.9 fs pulses spectrally centered at 780 nm. Pulses from the oscillator with 2 nJ energy are launched into a 1 mm long all-normal dispersive solid-core photonic crystal fiber and spectrally broadened to more than one octave. Subsequent pulse compression is achieved with a phase-only 4f pulse shaper. Second harmonic frequency resolved optical gating with a ptychographic reconstruction algorithm is used to obtain the spectral phase, which is fed back as a phase mask to the shaper display for pulse compression. The compressed pulses are CEP stable with a long term standard deviation of 0.23 rad for the CEP noise and 0.32 rad for the integrated rms phase jitter. The high total throughput of 15% results in a remaining pulse energy of about 300 pJ at 80 MHz repetition rate. With these parameters and the ability to tailor the spectral phase, the system is well suited for waveform sensitive photoemission experiments with needle tips or nanostructures and can be easily adapted to other sub-10 fs ultra-broadband Ti:sapphire oscillators.

Non-invasive real-time characterization of hollow-core photonic crystal fibers using whispering gallery mode spectroscopy.

Single-ring hollow-core photonic crystal fibers, consisting of a ring of one or two thin-walled glass capillaries surrounding a central hollow core, hold great promise for use in optical communications and beam delivery, and are already being successfully exploited for extreme pulse compression and efficient wavelength conversion in gases. However, achieving low loss over long (km) lengths requires highly accurate maintenance of the microstructure-a major fabrication challenge. In certain applications, for example adiabatic mode transformers, it is advantageous to taper the fibers, but no technique exists for measuring the delicate and complex microstructure without first cleaving the taper at several positions along its length. In this Letter, we present a simple non-destructive optical method for measuring the diameter of individual capillaries. Based on recording the spectrum scattered from whispering gallery modes excited in the capillary walls, the technique is highly robust, allowing real-time measurement of fiber structure during the draw with sub-micron accuracy.

Highly efficient deep UV generation by four-wave mixing in gas-filled hollow-core photonic crystal fiber.

We report on a highly efficient experimental scheme for the generation of deep-ultraviolet (UV) ultrashort light pulses using four-wave mixing in gas-filled kagomé-style photonic crystal fiber. By pumping with ultrashort, few microjoule pulses centered at 400 nm, we generate an idler pulse at 266 nm and amplify a seeded signal at 800 nm. We achieve remarkably high pump-to-idler energy conversion efficiencies of up to 38%. Although the pump and seed pulse durations are ∼100 fs, the generated UV spectral bandwidths support sub-15 fs pulses. These can be further extended to support few-cycle pulses. Four-wave mixing in gas-filled hollow-core fibers can be scaled to high average powers and different spectral regions such as the vacuum UV (100-200 nm).

Pulse-repetition-rate tuning of a harmonically mode-locked fiber laser using a tapered photonic crystal fiber.

Strong enhancement of optoacoustic interactions in the micrometer-sized core of a photonic crystal fiber (PCF) enables stable, harmonic mode locking of a soliton fiber laser at GHz frequencies. Here we report that by tapering the PCF during the draw, the optoacoustic gain bandwidth can be broadened to ∼47 MHz, more than 3 times wider than in the untapered fiber. This made possible broad pulse-repetition-rate tuning over 66 MHz (from 2.042 to 2.108 GHz) of an optoacoustically mode-locked soliton fiber laser. Within this tuning range, the harmonically mode-locked pulse trains at the laser output were observed to be quite robust, with better than 40 dB supermode suppression ratio, sub-ps pulse timing jitter, and <0.2%relative intensity noise. This gigahertz-rate, near-infrared soliton fiber laser has remarkable pulse-rate tunability and low noise level, and has important potential applications in frequency metrology, high-speed optical sampling, and fiber telecommunications.

Pump-probe multi-species CARS in a hollow-core PCF with a 20 ppm detection limit under ambient conditions.

We report coherent anti-Stokes Raman spectroscopy (CARS) in a gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF) using a pump-probe configuration. The long collinear path length offered by an SR-PCF strongly enhances the efficiency of the Raman interactions. Pressure tuning the zero-dispersion wavelength (ZDW) of the SR-PCF allows the Raman coherence prepared by seeded pumping at 515 nm to be used in the visible for phase-matched generation of an anti-Stokes signal from a probe in the ultraviolet. The unique dispersion profile in the vicinity of the ZDW enables simultaneous phase matching of all known Raman transitions. We demonstrate that simultaneous multi-species CARS with a detection limit of 20 ppm is possible with only 20 kW of peak pump power delivered by a single laser source.

Generation of broadband circularly polarized supercontinuum light in twisted photonic crystal fibers.

We compare the properties of the broadband supercontinuum (SC) generated in twisted and untwisted solid-core photonic crystal fibers when pumped by circularly polarized 40 picosecond laser pulses at 1064 nm. In the helically twisted fiber, fabricated by spinning the preform during the draw, the SC is robustly circularly polarized across its entire spectrum whereas, in the straight fiber, axial fluctuations in linear birefringence and polarization-dependent nonlinear effects cause the polarization state to vary randomly with the wavelength. Theoretical modelling confirms the experimental results. Helically twisted photonic crystal fibers permit the generation of pure circularly polarized SC light with excellent polarization stability against fluctuations in input power and environmental perturbations.

Carrier-envelope-phase-stable soliton-based pulse compression to 4.4 fs and ultraviolet generation at the 800 kHz repetition rate.

In this Letter, we report the generation of a femtosecond supercontinuum extending from the ultraviolet to the near-infrared spectrum and detection of its carrier-envelope-phase (CEP) variation by f-to-2f interferometry. The spectrum is generated in a gas-filled hollow-core photonic crystal fiber, where soliton dynamics allows the CEP-stable self-compression of the optical parametric chirped-pulse amplifier pump pulses at 800 nm to a duration of 1.7 optical cycles, followed by dispersive wave emission. The source provides up to 1 µJ of pulse energy at the 800 kHz repetition rate, resulting in 0.8 W of average power, and it can be extremely useful, for example in strong-field physics, pump-probe measurements, and ultraviolet frequency comb metrology.

Direct characterization of tuneable few-femtosecond dispersive-wave pulses in the deep UV.

Dispersive wave emission (DWE) in gas-filled hollow-core dielectric waveguides is a promising source of tuneable coherent and broadband radiation, but so far the generation of few-femtosecond pulses using this technique has not been demonstrated. Using in-vacuum frequency-resolved optical gating, we directly characterize tuneable 3 fs pulses in the deep ultraviolet generated via DWE. Through numerical simulations, we identify that the use of a pressure gradient in the waveguide is critical for the generation of short pulses.

Excitation of higher-order modes in optofluidic photonic crystal fiber.

Higher-order modes up to LP33 are controllably excited in water-filled kagomé- and bandgap-style hollow-core photonic crystal fibers (HC-PCF). A spatial light modulator is used to create amplitude and phase distributions that closely match those of the fiber modes, resulting in typical launch efficiencies of 10-20% into the liquid-filled core. Modes, excited across the visible wavelength range, closely resemble those observed in air-filled kagomé HC-PCF and match numerical simulations. Mode indices are obtained by launching plane-waves at specific angles onto the fiber input-face and comparing the resulting intensity pattern to that of a particular mode. These results provide a framework for spatially-resolved sensing in HC-PCF microreactors and fiber-based optical manipulation.