Mid-Infrared Frequency Comb Generation and Spectroscopy with Few-Cycle Pulses and χ

The mid-infrared atmospheric window of 3-5.5 µm holds valuable information regarding molecular composition and function for fundamental and applied spectroscopy. Using a robust, mode-locked fiber-laser source of <11 fs pulses in the near infrared, we explore quadratic (χ^{(2)}) nonlinear optical processes leading to frequency comb generation across this entire mid-infrared atmospheric window. With experiments and modeling, we demonstrate intrapulse difference frequency generation that yields few-cycle mid-infrared pulses in a single pass through periodically poled lithium niobate. Harmonic and cascaded χ^{(2)} nonlinearities further provide direct access to the carrier-envelope offset frequency of the near infrared driving pulse train. The high frequency stability of the mid-infrared frequency comb is exploited for spectroscopy of acetone and carbonyl sulfide with simultaneous bandwidths exceeding 11 THz and with spectral resolution as high as 0.003 cm^{-1}. The combination of low noise and broad spectral coverage enables detection of trace gases with concentrations in the part-per-billion range.

Efficient second harmonic generation in nanophotonic GaAs-on-insulator waveguides.

Nonlinear frequency conversion plays a crucial role in advancing the functionality of next-generation optical systems. Portable metrology references and quantum networks will demand highly efficient second-order nonlinear devices, and the intense nonlinear interactions of nanophotonic waveguides can be leveraged to meet these requirements. Here we demonstrate second harmonic generation (SHG) in GaAs-on-insulator waveguides with unprecedented efficiency of 40 W-1 for a single-pass device. This result is achieved by minimizing the propagation loss and optimizing phase-matching. We investigate surface-state absorption and design the waveguide geometry for modal phase-matching with tolerance to fabrication variation. A 2.0 µm pump is converted to a 1.0 µm signal in a length of 2.9 mm with a wide signal bandwidth of 148 GHz. Tunable and efficient operation is demonstrated over a temperature range of 45 °C with a slope of 0.24 nm/°C. Wafer-bonding between GaAs and SiO2 is optimized to minimize waveguide loss, and the devices are fabricated on 76 mm wafers with high uniformity. We expect this device to enable fully integrated self-referenced frequency combs and high-rate entangled photon pair generation.

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.

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.

Room-temperature-deposited dielectrics and superconductors for integrated photonics.

We present an approach to fabrication and packaging of integrated photonic devices that utilizes waveguide and detector layers deposited at near-ambient temperature. All lithography is performed with a 365 nm i-line stepper, facilitating low cost and high scalability. We have shown low-loss SiN waveguides, high-Q ring resonators, critically coupled ring resonators, 50/50 beam splitters, Mach-Zehnder interferometers (MZIs) and a process-agnostic fiber packaging scheme. We have further explored the utility of this process for applications in nonlinear optics and quantum photonics. We demonstrate spectral tailoring and octave-spanning supercontinuum generation as well as the integration of superconducting nanowire single photon detectors with MZIs and channel-dropping filters. The packaging approach is suitable for operation up to 160 °C as well as below 1 K. The process is well suited for augmentation of existing foundry capabilities or as a stand-alone process.

Platinum germanides for mid- and long-wave infrared plasmonics.

Platinum germanides (PtGe) were investigated for infrared plasmonic applications. Layers of Pt and Ge were deposited and annealed. X-ray diffraction identified PtGe(2) and Pt(2)Ge(3) phases, and x-ray photo-electron spectroscopy determined vertical atomic composition profiles for the films. Complex permittivity spectra were measured by ellipsometry over the 2 to 15 µm wavelength range. Surface plasmon polariton (SPP) characteristics such as propagation length and field penetration depth were calculated. Photon-to-SPP couplers in the form of 1D lamellar gratings were fabricated and characterized in the range 9 - 10.5 µm via wavelength-dependent specular reflection spectra for multiple angles of incidence. The observed resonances compare well with calculated spectra for SPP excitation on PtGe(2). Platinum germanides are CMOS compatible and may serve as SPP hosts for on-chip mid-IR plasmonic components with tighter field confinement than noble-metal hosts.