Sub-cycle pulse revealed with carrier-envelope phase control of soliton self-compression in anti-resonant hollow-core fiber.

The influence of the carrier-envelope phase (CEP) of a pump pulse on the multioctave supercontinuum (SC) generation in a gas-filled anti-resonant hollow-core fiber (AR HCF) by soliton self-compression (SSC) has been explored. We have shown an octave-wide third harmonic generation (THG) in the visible-to-near-infrared range during the pulse compression down to a sub-cycle duration. The CEP of a multi-cycle pump pulse provides control of interference between the third harmonic (TH) and the SC that indicates the coherent synthesis of a sub-cycle pulse with a duration of about 0.4 optical cycles and a peak power of more than 2 GW at the fiber output.

Multimodal nonlinear-optical imaging of nucleoli.

Multimodal nonlinear microscopy combining third-harmonic generation (THG) with two- and three-photon-excited fluorescence (2PEF and 3PEF) is shown to provide a powerful resource for high-fidelity imaging of nucleoli and nucleolar proteins. We demonstrate that, with a suitably tailored genetically encoded fluorescent stain, the 2PEF/3PEF readout from specific nucleolar proteins can be reliably detected against the extranucleolar 2PEF/3PEF signal, enabling high-contrast imaging of the key nucleolar ribosome biogenesis components, such as fibrillarin. THG is shown to provide a versatile readout for unstained nucleolus imaging in a vast class of biological systems as different as neurons in brain slices and cultured HeLa cells.

Cell-specific three-photon-fluorescence brain imaging: neurons, astrocytes, and gliovascular interfaces.

We present brain imaging experiments on rat cortical areas, demonstrating that, when combined with a suitable high-brightness, cell-specific genetically encoded fluorescent marker, three-photon-excited fluorescence (3PEF), enables subcellular-resolution, cell-specific 3D brain imaging that is fully compatible and readily integrable with other nonlinear-optical imaging modalities, including two-photon-fluorescence and harmonic-generation microscopy. With laser excitation provided by sub-100-fs, 1.25-µm laser pulses, cell-specific 3PEF from astrocytes and their processes detected in parallel with a three-photon-resonance-enhanced third harmonic from blood vessels is shown to enable a high-contrast 3D imaging of gliovascular interfaces.

Stain-free subcellular-resolution astrocyte imaging using third-harmonic generation.

We demonstrate stain-free, high-contrast, subcellular-resolution imaging of astroglial cells using epi-detected third-harmonic generation (THG). The astrocyte-imaging capability of THG is verified by colocalizing THG images with fluorescence images of astrocytes expressing a genetically encodable fluorescent reporter. We show that THG imaging with an optimized point-spread function can reliably detect significant subcellular features of astrocytes, including cell nuclei, as well as the soma shape and boundaries.

High-order harmonic analysis of anisotropic petahertz photocurrents in solids.

Polarization maps of high-order harmonics are shown to enable a full vectorial characterization of petahertz electron currents generated in a crystalline solid by an ultrashort laser driver. As a powerful resource of this methodology, analysis of energy-momentum dispersion landscapes, defined by the electron band structure, can help identify, as our analysis shows, special directions within the Brillouin zone that can provide a preferable basis for polarization-sensitive high-harmonic mapping of anisotropic petahertz photocurrents in solids.

Ultrafast mid-infrared spectrochronography of dispersion near molecular absorption bands.

Quantitative characterization of dispersion near molecular resonances is difficult both conceptually and technically, as it requires systematic measurements of rapidly varying dispersion profiles across the edges of molecular absorption bands. Here, we show that this challenge can be confronted with an ultrafast spectrochronography technique that combines time-resolved four-wave mixing and cross-correlation frequency-resolved optical gating. We demonstrate that, with the spectrum of an ultrashort mid-infrared laser probe stretching across the edge of a molecular absorption band, the Wigner chronocyclic maps of such a probe reveal universal signatures of anomalous dispersion and help quantify such dispersion anomalies.

Fiber-optic electron-spin-resonance thermometry of single laser-activated neurons.

Optically detected electron spin resonance in fiber-coupled nitrogen-vacancy (NV) centers of diamond is used to demonstrate a fiber-optic quantum thermometry of individual thermogenetically activated neurons. Laser-induced temperature variations read out from single neurons with the NV-diamond fiber sensor are shown to strongly correlate with the fluorescence of calcium-ion sensors, serving as online indicators of the inward Ca2+ current across the cell membrane of neurons expressing transient receptor potential (TRP) cation channels. Local laser heating above the TRP-channel activation threshold is shown to reproducibly evoke robust action potentials, visualized by calcium-ion-sensor-aided fluorescence imaging and detected as prominent characteristic waveforms in the time-resolved response of fluorescence Ca2+ sensors.

Modeling high-peak-power few-cycle field waveform generation by optical parametric amplification in the long-wavelength infrared.

Extended coupled-wave analysis of optical parametric chirped-pulse amplification (OPCPA) reveals regimes whereby high-peak-power few-cycle pulses can be generated in the long-wavelength infrared (LWIR) spectral range. Broadband OPCPA in suitable nonlinear crystals pumped at around 2 µm and seeded either through the signal or the idler input is shown to enable the generation of high-power field waveforms with pulse widths shorter than two field cycles within the entire LWIR range.

Solid-State Source of Subcycle Pulses in the Midinfrared.

We demonstrate a robust, all-solid-state approach for the generation of microjoule subcycle pulses in the midinfrared through a cascade of carefully optimized parametric-amplification, difference-frequency-generation, spectral-broadening, and chirp-compensation stages. This method of subcycle waveform generation becomes possible due to an unusual, ionization-assisted solid-state pulse self-compression dynamics, where highly efficient spectral broadening is enabled by ultrabroadband four-wave parametric amplification phase matched near the zero-group-velocity wavelength of the material.

Stimulated Raman gas sensing by backward UV lasing from a femtosecond filament.

We perform a proof-of-principle demonstration of chemically specific standoff gas sensing, in which a coherent stimulated Raman signal is detected in the direction anticollinear to a two-color laser excitation beam traversing the target volume. The proposed geometry is intrinsically free space as it does not involve back-scattering (reflection) of the signal or excitation beams at or behind the target. A beam carrying an intense mid-IR femtosecond (fs) pulse and a parametrically generated picosecond (ps) UV Stokes pulse is fired in the forward direction. A fs filament, produced by the intense mid-IR pulse, emits a backward-propagating narrowband ps laser pulse at the 337 and 357 nm transitions of excited molecular nitrogen, thus supplying a counter-propagating Raman pump pulse. The scheme is linearly sensitive to species concentration and provides both transverse and longitudinal spatial resolution.

Multioctave, 3-18 µm sub-two-cycle supercontinua from self-compressing, self-focusing soliton transients in a solid.

Strongly coupled nonlinear spatiotemporal dynamics of ultrashort mid-infrared pulses undergoing self-focusing simultaneously with soliton self-compression in an anomalously dispersive, highly nonlinear solid semiconductor is shown to enable the generation of multioctave supercontinua with spectra spanning the entire mid-infrared range and compressible to subcycle pulse widths. With 7.9 µm, 150 fs, 2 µJ, 1 kHz pulses used as a driver, 1.2 cycle pulses of mid-infrared supercontinuum radiation with a spectrum spanning the range of wavelengths from 3 to 18 µm were generated in a 5 mm GaAs plate. Further compression of these pulses to subcycle pulse widths is possible through compensation of the residual phase shift.

Frequency-tunable sub-two-cycle 60-MW-peak-power free-space waveforms in the mid-infrared.

A physical scenario whereby freely propagating mid-infrared pulses can be compressed to pulse widths close to the field cycle is identified. Generation of tunable few-cycle pulses in the wavelength range from 4.2 to 6.8 µm is demonstrated at a 1-kHz repetition rate through self-focusing-assisted spectral broadening in a normally dispersive, highly nonlinear semiconductor material, followed by pulse compression in the regime of anomalous dispersion, where the dispersion-induced phase shift is finely tuned by adjusting the overall thickness of anomalously dispersive components. Sub-two-cycle pulses with a peak power up to 60 MW are generated in the range of central wavelengths tunable from 5.9 to 6.3 µm.

Time-domain spectroscopy in the mid-infrared.

When coupled to characteristic, fingerprint vibrational and rotational motions of molecules, an electromagnetic field with an appropriate frequency and waveform offers a highly sensitive, highly informative probe, enabling chemically specific studies on a broad class of systems in physics, chemistry, biology, geosciences, and medicine. The frequencies of these signature molecular modes, however, lie in a region where accurate spectroscopic measurements are extremely difficult because of the lack of efficient detectors and spectrometers. Here, we show that, with a combination of advanced ultrafast technologies and nonlinear-optical waveform characterization, time-domain techniques can be advantageously extended to the metrology of fundamental molecular motions in the mid-infrared. In our scheme, the spectral modulation of ultrashort mid-infrared pulses, induced by rovibrational motions of molecules, gives rise to interfering coherent dark waveforms in the time domain. These high-visibility interference patterns can be read out by cross-correlation frequency-resolved gating of the field in the visible generated through ultrabroadband four-wave mixing in a gas phase.

Pulse-width-tunable 0.7 W mode-locked Cr: forsterite laser.

A mode-locked chromium forsterite laser with output power in excess of 0.7 W, a central wavelength of 1.25 µm, a pulse repetition rate of 29 MHz, and an output pulse-width-tunable from 40 to 200 fs is demonstrated. The dynamics behind the buildup of ultrashort light pulses in this laser is shown to involve spectral and temporal breathing due to the interplay of gain, Kerr nonlinearity, and dispersion effects. The pulse-width-tunable 1.25 µm output delivered by the developed laser source suggests a powerful tool for nonlinear-optical bio-imaging and offers an advantageous front end for extreme-power laser technologies.

The phase-controlled Raman effect.

Unlike spontaneous Raman effect, nonlinear Raman scattering generates fields with a well-defined phase, allowing Raman signals from individual scatterers to add up into a highly directional, high-brightness coherent beam. Here, we show that the phase of coherent Raman scattering can be accurately controlled and finely tuned by using spectrally and temporally tailored optical driver fields. In our experiments, performed with spectrally optimized phase-tunable laser pulses, such a phase control is visualized through the interference of the coherent Raman signal with the field resulting from nonresonant four-wave mixing. This interference gives rise to Fano-type profiles in the overall nonlinear response measured as a function of the delay time between the laser pulses, featuring a well-resolved destructive-interference dip on the dark side of the Raman peak. This phase-control strategy is shown to radically enhance the coherent response from weak Raman modes, thus helping confront long-standing challenges in nonlinear Raman imaging and microspectroscopy.

Ultrafast-laser-induced backward stimulated Raman scattering for tracing atmospheric gases.

By combining tunable broadband pulse generation with the technique of nonlinear spectral compression we demonstrate a prototype scheme for highly selective detection of air molecules by backward stimulated Raman scattering. The experimental results allow to extrapolate the laser parameters required for standoff sensing based on the recently demonstrated backward atmospheric lasing.

Stimulated Raman amplification and high-order Raman sideband generation in a polymer waveguide on a printed circuit.

The ultrafast Raman response of C-H vibrations in polymer waveguides on a printed circuit is shown to enable a high-gain amplification and high-order stimulated Raman transformation of ultrashort laser pulses. The pump and Stokes fields coupled by the C-H vibration mode with a vibration cycle of 11 fs give rise to multiple Raman sidebands, suggesting the way toward ultrafast optical data processing and few-cycle optical waveform synthesis on a printed-circuit polymer waveguide platform.

Coherent anti-Stokes Raman metrology of phonons powered by photonic-crystal fibers.

Coherent anti-Stokes Raman scattering (CARS) is used to measure the amplitude, the dephasing lifetime, and parameters of optical nonlinearities of optical phonons in a synthetic diamond film. A compact CARS apparatus demonstrated in this work relies on the use of an unamplified 70 fs 340 mW Cr:forsterite laser output and photonic-crystal fibers optimized for the generation of wavelength-tunable Stokes field and the spectral compression of the probe pulse.