Direct Observation of Enhanced Electron-Phonon Coupling in Copper Nanoparticles in the Warm-Dense Matter Regime.

Warm dense matter (WDM) represents a highly excited state that lies at the intersection of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. In this work, by exciting isolated ∼8 nm copper nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly excited WDM. Using photoelectron spectroscopy, we measure the instantaneous electron temperature and extract the electron-ion coupling of the nanoparticle as it undergoes a solid-to-WDM phase transition. By comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by a fast energy loss of electrons to ions, and a strong modulation of the electron temperature induced by strong acoustic breathing modes that change the nanoparticle volume. This work demonstrates a new route for experimental exploration of the exotic properties of WDM.

Bright, single helicity, high harmonics driven by mid-infrared bicircular laser fields.

High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8 µm and 2.0 µm to extend the photon energy range of circularly polarized high-harmonics and also generate single-helicity HHG spectra. By driving HHG in helium, we produce circularly polarized soft x-ray harmonics beyond 170 eV-the highest photon energy of circularly polarized HHG achieved to date. In an Ar medium, dense spectra at photon energies well beyond the Cooper minimum are generated, with regions composed of a single helicity-consistent with the generation of a train of circularly polarized attosecond pulses. Finally, we show theoretically that circularly polarized HHG photon energies can extend beyond the carbon K edge, extending the range of molecular and materials systems that can be accessed using dynamic HHG chiral spectro-microscopies.

Broadband, electro-optic, dual-comb spectrometer for linear and nonlinear measurements.

We demonstrate a dual-comb spectrometer based on electro-optic modulation of a continuous-wave laser at 10 GHz. The system simultaneously offers fast acquisition speed and ultrabroad spectral coverage, spanning 120 THz across the near infrared. Our spectrometer is highly adaptable, and we demonstrate absorption spectroscopy of atmospheric gases and a dual-comb configuration that captures nonlinear Raman spectra of semiconductor materials via coherent anti-Stokes Raman scattering. The ability to rapidly and simultaneously acquire broadband spectra with high frequency resolution and high sensitivity points to new possibilities for hyperspectral sensing in fields such as remote sensing, biological detection and imaging, and machine vision.

Mid-infrared frequency combs at 10 GHz.

We demonstrate mid-infrared (MIR) frequency combs at 10 GHz repetition rate via intra-pulse difference-frequency generation (DFG) in quasi-phase-matched nonlinear media. Few-cycle pump pulses (≲15fs, 100 pJ) from a near-infrared electro-optic frequency comb are provided via nonlinear soliton-like compression in photonic-chip silicon-nitride waveguides. Subsequent intra-pulse DFG in periodically poled lithium niobate waveguides yields MIR frequency combs in the 3.1-4.8 µm region, while orientation-patterned gallium phosphide provides coverage across 7-11 µm. Cascaded second-order nonlinearities simultaneously provide access to the carrier-envelope-offset frequency of the pump source via in-line f-2f nonlinear interferometry. The high-repetition rate MIR frequency combs introduced here can be used for condensed phase spectroscopy and applications such as laser heterodyne radiometry.

Generating few-cycle pulses with integrated nonlinear photonics.

Ultrashort laser pulses that last only a few optical cycles have been transformative tools for studying and manipulating light-matter interactions. Few-cycle pulses are typically produced from high-peak-power lasers, either directly from a laser oscillator or through nonlinear effects in bulk or fiber materials. Now, an opportunity exists to explore the few-cycle regime with the emergence of fully integrated nonlinear photonics. Here, we experimentally and numerically demonstrate how lithographically patterned waveguides can be used to generate few-cycle laser pulses from an input seed pulse. Moreover, our work explores a design principle in which lithographically varying the group-velocity dispersion in a waveguide enables the creation of highly constant-intensity supercontinuum spectra across an octave of bandwidth. An integrated source of few-cycle pulses could broaden the range of applications for ultrafast light sources, including supporting new lab-on-a-chip systems in a scalable form factor.

Dual-comb spectroscopy with tailored spectral broadening in Si3N4 nanophotonics.

Si3N4 waveguides, pumped at 1550 nm, can provide spectrally smooth, broadband light for gas spectroscopy in the important 2 µm to 2.5 µm atmospheric water window, which is only partially accessible with silica-fiber based systems. By combining Er+ fiber frequency combs and supercontinuum generation in tailored Si3N4 waveguides, high signal-to-noise dual-comb spectroscopy spanning 2 µm to 2.5 µm is demonstrated. Acquired broadband dual-comb spectra of CO and CO2 agree well with database line shape models and have a spectral-signal-to-noise as high as 48/√s, showing that the high coherence between the two combs is retained in the Si3N4 supercontinuum generation. The dual-comb spectroscopy figure of merit is 6 × 106/√s, equivalent to that of all-fiber dual-comb spectroscopy systems in the 1.6 µm band. based on these results, future dual-comb spectroscopy can combine fiber comb technology with Si3N4 waveguides to access new spectral windows in a robust non-laboratory platform.

Dual-comb interferometry via repetition rate switching of a single frequency comb.

We experimentally demonstrate a versatile technique for performing dual-comb interferometry using a single frequency comb. By rapid switching of the repetition rate, the output pulse train can be delayed and heterodyned with itself to produce interferograms. The full speed and resolution of standard dual-comb interferometry is preserved while simultaneously offering a significant experimental simplification and cost savings. We show that this approach is particularly suited for absolute distance metrology due to an extension of the nonambiguity range as a result of the continuous repetition rate switching.

Tunable mid-infrared generation via wide-band four-wave mixing in silicon nitride waveguides.

We demonstrate wide-band frequency down-conversion to the mid-infrared (MIR) using four-wave mixing (FWM) of near-infrared (NIR) femtosecond-duration pulses from an Er:fiber laser, corresponding to 100 THz spectral translation. Photonic-chip-based silicon nitride waveguides provide the FWM medium. Engineered dispersion in the nanophotonic geometry and the wide transparency range of silicon nitride enable large-detuning FWM phase-matching and results in tunable MIR from 2.6 to 3.6 µm on a single chip with 100-pJ-scale pump-pulse energies. Additionally, we observe up to 25 dB broadband parametric gain for NIR pulses when the FWM process is operated in a frequency up-conversion configuration. Our results demonstrate how integrated photonic circuits pumped with fiber lasers could realize multiple nonlinear optical phenomena on the same chip and lead to engineered synthesis of broadband, tunable, and coherent light across the NIR and MIR wavelength bands.

Mid-infrared frequency comb generation via cascaded quadratic nonlinearities in quasi-phase-matched waveguides.

We experimentally demonstrate a simple configuration for mid-infrared (MIR) frequency comb generation in quasi-phase-matched lithium niobate waveguides using the cascaded-χ(2) nonlinearity. With nanojoule-scale pulses from an Er:fiber laser, we observe octave-spanning supercontinuum in the near-infrared with dispersive wave generation in the 2.5-3 µm region and intrapulse difference frequency generation in the 4-5 µm region. By engineering the quasi-phase-matched grating profiles, tunable, narrowband MIR and broadband MIR spectra are both observed in this geometry. Finally, we perform numerical modeling using a nonlinear envelope equation, which shows good quantitative agreement with the experiment-and can be used to inform waveguide designs to tailor the MIR frequency combs. Our results identify a path to a simple single-branch approach to mid-infrared frequency comb generation in a compact platform using commercial Er:fiber technology.

Deuterated silicon nitride photonic devices for broadband optical frequency comb generation.

We report and characterize low-temperature, plasma-deposited deuterated silicon nitride films for nonlinear integrated photonics. With a peak processing temperature less than 300°C, it is back-end compatible with complementary metal-oxide semiconductor substrates. We achieve microresonators with a quality factor of up to 1.6×106 at 1552 nm and >1.2×106 throughout λ=1510-1600 nm, without annealing or stress management (film thickness of 920 nm). We then demonstrate the immediate utility of this platform in nonlinear photonics by generating a 1 THz free-spectral-range, 900 nm bandwidth modulation-instability microresonator Kerr comb and octave-spanning, supercontinuum-broadened spectra.

Quasi-Phase-Matched Supercontinuum Generation in Photonic Waveguides.

Supercontinuum generation (SCG) in integrated photonic waveguides is a versatile source of broadband light, and the generated spectrum is largely determined by the phase-matching conditions. Here we show that quasi-phase-matching via periodic modulations of the waveguide structure provides a useful mechanism to control the evolution of ultrafast pulses during supercontinuum generation. We experimentally demonstrate a quasi-phase-matched supercontinuum to the TE_{20} and TE_{00} waveguide modes, which enhances the intensity of the SCG in specific spectral regions by as much as 20 dB. We utilize higher-order quasi-phase-matching (up to the 16th order) to enhance the intensity in numerous locations across the spectrum. Quasi-phase-matching adds a unique dimension to the design space for SCG waveguides, allowing the spectrum to be engineered for specific applications.

Bright circularly polarized soft X-ray high harmonics for X-ray magnetic circular dichroism.

We demonstrate, to our knowledge, the first bright circularly polarized high-harmonic beams in the soft X-ray region of the electromagnetic spectrum, and use them to implement X-ray magnetic circular dichroism measurements in a tabletop-scale setup. Using counterrotating circularly polarized laser fields at 1.3 and 0.79 µm, we generate circularly polarized harmonics with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right circularly polarized peaks, with energies determined by conservation of energy and spin angular momentum. We explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase-matching conditions. The first advanced phase-matched propagation simulations for circularly polarized harmonics reveal the influence of the finite phase-matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. Finally, we use, to our knowledge, the first tabletop X-ray magnetic circular dichroism measurements at the N4,5 absorption edges of Gd to validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum, and temporal shape of high harmonics in the soft X-ray region by manipulating the driving laser waveform.

Phase matching of noncollinear sum and difference frequency high harmonic generation above and below the critical ionization level.

We investigate the macroscopic physics of noncollinear high harmonic generation (HHG) at high pressures. We make the first experimental demonstration of phase matching of noncollinear high-order-difference-frequency generation at ionization fractions above the critical ionization level, which normally sets an upper limit on the achievable cutoff photon energies. Additionally, we show that noncollinear high-order-sum-frequency generation requires much higher pressures for phase matching than single-beam HHG does, which mitigates the short interaction region in this geometry. We also dramatically increase the experimentally realized cutoff energy of noncollinear circularly polarized HHG, reaching photon energies of 90 eV. Finally, we achieve complete angular separation of high harmonic orders without the use of a spectrometer.

Self-referenced frequency combs using high-efficiency silicon-nitride waveguides.

We utilize silicon-nitride waveguides to self-reference a telecom-wavelength fiber frequency comb through supercontinuum generation, using 11.3 mW of optical power incident on the chip. This is approximately 10 times lower than conventional approaches using nonlinear fibers and is enabled by low-loss (<2 dB) input coupling and the high nonlinearity of silicon nitride, which can provide two octaves of spectral broadening with incident energies of only 110 pJ. Following supercontinuum generation, self-referencing is accomplished by mixing 780-nm dispersive-wave light with the frequency-doubled output of the fiber laser. In addition, at higher optical powers, we demonstrate f-to-3f self-referencing directly from the waveguide output by the interference of simultaneous supercontinuum and third harmonic generation, without the use of an external doubling crystal or interferometer. These hybrid comb systems combine the performance of fiber-laser frequency combs with the high nonlinearity and compactness of photonic waveguides, and should lead to low-cost, fully stabilized frequency combs for portable and space-borne applications.

Helicity-Selective Enhancement and Polarization Control of Attosecond High Harmonic Waveforms Driven by Bichromatic Circularly Polarized Laser Fields.

High harmonics driven by two-color counterrotating circularly polarized laser fields are a unique source of bright, circularly polarized, extreme ultraviolet, and soft x-ray beams, where the individual harmonics themselves are completely circularly polarized. Here, we demonstrate the ability to preferentially select either the right or left circularly polarized harmonics simply by adjusting the relative intensity ratio of the bichromatic circularly polarized driving laser field. In the frequency domain, this significantly enhances the harmonic orders that rotate in the same direction as the higher-intensity driving laser. In the time domain, this helicity-dependent enhancement corresponds to control over the polarization of the resulting attosecond waveforms. This helicity control enables the generation of circularly polarized high harmonics with a user-defined polarization of the underlying attosecond bursts. In the future, this technique should allow for the production of bright highly elliptical harmonic supercontinua as well as the generation of isolated elliptically polarized attosecond pulses.

Lorentz drift compensation in high harmonic generation in the soft and hard X-ray regions of the spectrum.

We present a semi-classical study of the effects of the Lorentz force on electrons during high harmonic generation in the soft and hard X-ray regions driven by near- and mid-infrared lasers with wavelengths from 0.8 to 20 µm, and at intensities below 1015 W/cm2. The transverse extent of the longitudinal Lorentz drift is compared for both Gaussian focus and waveguide geometries. Both geometries exhibit a longitudinal electric field component that cancels the magnetic Lorentz drift in some regions of the focus, once each full optical cycle. We show that the Lorentz force contributes a super-Gaussian scaling which acts in addition to the dominant high harmonic flux scaling of λ-(5-6) due to quantum diffusion. We predict that the high harmonic yield will be reduced for driving wavelengths > 6 µm, and that the presence of dynamic spatial mode asymmetries results in the generation of both even and odd harmonic orders. Remarkably, we show that under realistic conditions, the recollision process can be controlled and does not shut off completely even for wavelengths >10 µm and recollision energies greater than 15 keV.

Dynamics of Strong-Field Double Ionization in Two-Color Counterrotating Fields.

The double ionization of helium in bichromatic, circularly polarized intense laser fields is analyzed with a classical ensemble approach. It is found that counterrotating fields produce significant nonsequential double-ion yield and drive novel ionization dynamics. It is shown that distinct pathways to ionization can be modified by altering the relative intensities of the two colors, allowing for unique control of strong-field processes. Electrons are observed to return to the ion at different angles from the angle of ionization, opening new possibilities for probing electronic and molecular structure on the ultrafast time scale.

Controlling Nonsequential Double Ionization in Two-Color Circularly Polarized Femtosecond Laser Fields.

Atoms undergoing strong-field ionization in two-color circularly polarized femtosecond laser fields exhibit unique two-dimensional photoelectron trajectories and can emit bright circularly polarized extreme ultraviolet and soft-x-ray beams. In this Letter, we present the first experimental observation of nonsequential double ionization in these tailored laser fields. Moreover, we can enhance or suppress nonsequential double ionization by changing the intensity ratio and helicity of the two driving laser fields to maximize or minimize high-energy electron-ion rescattering. Our experimental results are explained through classical simulations, which also provide insight into how to optimize the generation of circularly polarized high harmonic beams.

Solvents effects on charge transfer from quantum dots.

To predict and understand the performance of nanodevices in different environments, the influence of the solvent must be explicitly understood. In this Communication, this important but largely unexplored question is addressed through a comparison of quantum dot charge transfer processes occurring in both liquid phase and in vacuum. By comparing solution phase transient absorption spectroscopy and gas-phase photoelectron spectroscopy, we show that hexane, a common nonpolar solvent for quantum dots, has negligible influence on charge transfer dynamics. Our experimental results, supported by insights from theory, indicate that the reorganization energy of nonpolar solvents plays a minimal role in the energy landscape of charge transfer in quantum dot devices. Thus, this study demonstrates that measurements conducted in nonpolar solvents can indeed provide insight into nanodevice performance in a wide variety of environments.

High flux coherent super-continuum soft X-ray source driven by a single-stage, 10mJ, Ti:sapphire amplifier-pumped OPA.

We demonstrate the highest flux tabletop source of coherent soft X-rays to date, driven by a single-stage 10 mJ Ti:sapphire regenerative amplifier at 1 kHz. We first down-convert the laser to 1.3 µm using a parametric amplifier, before up-converting it to soft X-rays using high harmonic generation in a high-pressure, phase matched, hollow waveguide geometry. The resulting optimally phase matched broadband spectrum extends to 200 eV, with a soft X-ray photon flux of > 10(6) photons/pulse/1% bandwidth at 1 kHz, corresponding to > 10(9) photons/s/1% bandwidth, or approximately a three order-of-magnitude increase compared with past work. Finally, using this broad bandwidth X-ray source, we demonstrate X-ray absorption spectroscopy of multiple elements and transitions in molecules in a single spectrum, with a spectral resolution of 0.25 eV, and with the ability to resolve the near edge fine structure.