Long-term stabilization of carrier envelope phases of mid-infrared pulses for the precise detection of phase-sensitive responses to electromagnetic waves
T. Yamakawa, N. Sono, T. Kitao, T. Morimoto, N. Kida, T. Miyamoto, H. Okamoto
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17 pages including 4 figures (Supplementary materials: 4 pages including no figures)
We report a newly designed mid-infrared-pump visible-probe measurement system, which can measure phase-sensitive responses to a mid-infrared pulse along the oscillating electromagnetic field. In this system, the pump light is a phase-locked mid-infrared pulse with temporal width of 100 fs, which is produced via difference frequency generation (DFG) from two idler pulses of two optical parametric amplifiers (OPAs) that are excited by the same Ti:sapphire regenerative amplifier. The probe pulse is a visible pulse with temporal width of 9 fs, and it is generated from a custom-built non-collinear OPA. By measuring the electric-field waveforms of mid-infrared pump pulses with electro-optic sampling and evaluating their carrier envelope phase (CEP) and the temporal positions of their envelopes relative to ultrashort visible probe pulses, we are able to perform double feedback corrections that eliminate both the following sources of drift. The CEP drift in mid-infrared pulses originating from fluctuations in the difference of optical-path lengths of the two idler pulses before the DFG is corrected by inserting a wedge plate in one idler path, and the drift in pump-probe delay times due to fluctuations in the difference of the overall optical-path lengths of the pump and probe pulses is corrected with mechanical delay lines. In this double-feedback system, the absolute carrier phase of mid-infrared pulses can be fixed within 200 mrad and errors in the measurement of phase-sensitive responses can be reduced to within 1 fs over a few tens of hours.
Controlling the carrier envelope phase (CEP) in mode-locked lasers over practically long timescales is crucial for real-world applications in ultrafast optics and precision metrology. We present a hybrid solution that combines a feed-forward technique to stabilize the phase offset in fast timescales and a feedback technique that addresses slowly varying sources of interference and locking bandwidth limitations associated with gain media with long upper-state lifetimes. We experimentally realize the hybrid stabilization system in an Er:Yb:glass mode-locked laser and demonstrate 75 hours of stab…
Carrier-envelope phase stabilization of optical pulses enables exquisitely precise measurements by way of direct optical-frequency synthesis, absolute optical-to-microwave phase conversion, and control of ultrafast waveforms. We report such phase stabilization for Kerr-microresonator frequency combs integrated on silicon chips, and verify their fractional-frequency inaccuracy at <3x10-16. Our work introduces an interlocked Kerr-comb configuration comprised of one silicon-nitride and one silica microresonator, which feature nearly harmonic repetition frequencies and can be generated with one la…
Few-cycle pulsed laser technology highlights the need for control and stabilization of the carrier-envelope phase (CEP) for applications requiring shot-to-shot timing and phase consistency. This general requirement has been achieved successfully in a number of free space and fiber lasers via feedback and feed-forward methods. Expanding upon existing results, we demonstrate CEP stabilization through the feed-forward method applied to a SESAM mode-locked Er:Yb:glass laser at 1.55 um with a measured ultralow timing jitter of 2.9 as (1 Hz - 3 MHz) and long-term stabilization over a duration of eig…
We stabilize the idler frequency of a singly-resonant optical parametric oscillator directly to the resonance of a mid-infrared Fabry-Pérot reference cavity. This is accomplished by the Pound-Drever-Hall locking scheme, controlling either the pump laser or the resonant signal frequency. A residual relative frequency noise power spectral density below 10$^3$ Hz$^2$/Hz is reached, with a Gaussian linewidth of 920 Hz over 100 ms, which demonstrates the potential for reaching spectral purity down to the Hz level by locking the optical parametric oscillator against a mid-infrared cavity with state-…
We demonstrate an active carrier-envelope phase (CEP) stabilization scheme for optical waveforms generated by difference-frequency mixing of two spectrally detuned and phase-correlated pulses. By performing ellipsometry with spectrally overlapping parts of two co-propagating near-infrared generation pulse trains, we stabilize their relative timing to 18 as. Consequently, we can lock the CEP of the generated mid-infrared (MIR) pulses with a remaining phase jitter below 30 mrad. Employing these pulses for high-harmonic generation in a bulk semiconductor validates our technique. This experiment r…
A robust method for producing half-cycle - few-cycle pulses in mid-infrared to extreme ultraviolet spectral ranges is proposed. It is based on coherent undulator radiation of relativistic ultrathin electron layers, which are produced by microbunching of ultrashort electron bunches by a TW power laser in a modulator undulator. According to our numerical calculations it is possible to generate as short as 10 nm long electron layers in a single-period modulator undulator having an undulator parameter of only K=0.25 and which is significantly shorter than the resonant period length. By using these…
We experimentally demonstrate in a difference-frequency generation mid-infrared frequency comb source the effect of temporal overlap between pump- and signal- pulse to the relative intensity noise (RIN) of the idler pulse. When scanning the temporal delay between our 130 fs long signal- and pump pulses, we observe a RIN minimum with a 3 dB width of 20 fs delay and an RIN increase of 20 dB in 40 fs delay at the edges of this minimum. We also demonstrate active long-term stabilization of the mid-infrared frequency comb source to the temporal overlap setting corresponding to the lowest RIN operat…
Mid-infrared laser frequency combs are compelling sources for precise and sensitive metrology with applications in molecular spectroscopy and spectro-imaging. The infrared atmospheric window between 3-5.5 $μ$m in particular provides vital information regarding molecular composition. Using a robust, fiber-optic source of few-cycle pulses in the near-infrared, we experimentally demonstrate ultra-broad bandwidth nonlinear phenomena including harmonic and difference frequency generation in a single pass through periodically poled lithium niobate (PPLN). These $χ^{(2)}$ nonlinear optical processes …
We demonstrate a robust and simple method for measurement, stabilization and tuning of the frequency of cw mid-infrared (MIR) lasers, in particular of quantum cascade lasers. The proof of principle is performed with a quantum cascade laser at 5.4 μm, which is upconverted to 1.2 μm by sum-frequency generation in orientation-patterned GaAs with the output of a standard high-power cw 1.5 μm fiber laser. Both the 1.2 μm and the 1.5 μm waves are measured by a standard Er:fiber frequency comb. Frequency measurement at the 100 kHz-level, stabilization to sub-10 kHz level, controlled frequency tuning …
Based on the dual-chirped optical parametric amplification and type-I BiB$_3$O$_6$(BiBO) crystals, the generation of $>$100 mJ, 10.4 fs, 10 Hz, carrier-to-envelope phase (CEP)-stable laser pulses, which are centered at 1.7 $μ$m, is demonstrated; it produces a peak power of 10 TW. CEP-dependent high harmonic generation is implemented to confirm the sub-two-cycle pulse duration and CEP stabilization of infrared (IR) laser pulses. As far as we know, the obtained pulse energy and peak power represent the highest values for sub-two-cycle CEP-stable IR optical parametric amplification. Additionally,…
We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fountain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $μ$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabi…
This paper shows the experimental details of the stabilization scheme that allows full control of the repetition rate and the carrier-envelope offset frequency of a 10 GHz frequency comb based on a femtosecond Ti:sapphire laser. Octave-spanning spectra are produced in nonlinear microstructured optical fiber, in spite of the reduced peak power associated with the 10 GHz repetition rate. Improved stability of the broadened spectrum is obtained by temperature-stabilization of the nonlinear optical fiber. The carrier-envelope offset frequency and the repetition rate are simultaneously frequency st…
We investigated the carrier-envelope phase (CEP) stability of a hollow-fiber setup used for high-energy, few-cycle pulse generation. Saturation of the output pulse energy is observed at 0.6 mJ for a 260 um inner-diameter, 1 m long fiber, statically filled with neon, with the pressure adjusted to achieve an output spectrum capable of supporting sub-4fs pulses. The maximum output pulse energy can be increased to 0.8mJ by using either differential pumping, or circularly polarized input pulses. We observe the onset of an ionization-induced CEP instability, which does not increase beyond an input p…
Frequency-stabilized mid-infrared lasers are valuable tools for precision molecular spectroscopy. However, their implementation remains limited by complicated stabilization schemes. Here we achieve optical self-locking of a quantum cascade laser to the resonant leak-out field of a highly mode-matched two-mirror cavity. The result is a simple approach to achieving ultra-pure frequencies from high-powered mid-infrared lasers. For short time scales (<0.1 ms), we report a linewidth reduction factor of $3\times10^{-6}$ to a linewidth of 12 Hz. Furthermore, we demonstrate two-photon cavity-enhanced …
We demonstrate mid-infrared (mid-IR) supercontinuum generation (SCG) with instantaneous bandwidth from 2.2 to 5 μm at 40 dB below the peak, covering the wavelength range desirable for molecular spectroscopy and numerous other applications. The SCG occurs in a tapered As2S3 fiber prepared by in-situ tapering and is pumped by femtosecond pulses from the subharmonic of a mode-locked Er-doped fiber laser. Interference with a narrow linewidth c.w. laser verifies that the coherence properties of the near-IR frequency comb have been preserved through these cascaded nonlinear processes. With this appr…
Mid-infrared (mid-IR) frequency combs have broad applications in molecular spectroscopy and chemical/biological sensing. Recently developed microresonator-based combs in this wavelength regime could enable portable and robust devices using a single-frequency pump field. Here, we report the first demonstration of a modelocked microresonator-based frequency comb in the mid-IR spanning 2.4 μm to 4.3 μm. We observe high pump-to-comb conversion efficiency, in which 40% of the pump power is converted to the output comb power. Utilizing an integrated PIN structure allows for tuning the silicon micror…
We numerically study, by means of the single envelope equation, the generation of optical frequency combs ranging from the visible to the mid-infrared spectral regions in resonators with quadratic and cubic nonlinearities. Phase-matched quadratic wave-mixing processes among the comb lines can be activated by low-power continuous wave pumping in the near infrared of a radially poled lithium niobate whispering gallery resonator (WGR). We examine both separate and co-existing intra-cavity doubly resonant second-harmonic generation and parametric oscillation processes, and find that modulation ins…
The measurement and stabilization of the carrier-envelope offset frequency $f_{\textrm{CEO}}$ via self-referencing is paramount for optical frequency comb generation which has revolutionized precision frequency metrology, spectroscopy, and optical clocks. Over the past decade, the development of chip-scale platforms has enabled compact integrated waveguides for supercontinuum generation. However, there is a critical need for an on-chip self-referencing system that is adaptive to different pump wavelengths, requires low pulse energy, and does not require complicated processing. Here, we demonst…
We demonstrate the use of a flexible digital servo system for the optical stabilization of both the repetition rate and carrier-envelope offset frequency of a laser frequency comb. The servo system is based entirely on a low-cost field programmable gate array, simple electronic components, and existing open-source software. Utilizing both slow and fast feedback actuators of a commercial mode-locked laser frequency comb, we maintain cycle-slip free locking of optically-derived beatnotes over a 30 hour period, and measure residual phase noise at or below ~0.1 rad, corresponding to <100 attosecon…
BGGSe is a newly developed nonlinear material that is attractive for ultrabroad frequency mixing and ultrashort pulse generation due to its comparably low dispersion and high damage threshold.In a first experiment, we show that a long crystal length of 2.6 mm yields a pulse energy of 21 pJ at 100 MHz with a spectral bandwidth covering 5.8 to 8.5 microns. The electric field of the carrier-envelope-phase stable pulse is directly measured with electro-optical sampling and reveals a pulse duration of 91 fs, which corresponds to sub-four optical cycles, thus confirming some of the prospects of the …
Carrier-envelope phase (CEP) detection of ultrashort optical pulses and low-energy waveform field sampling have recently been demonstrated using direct time-domain methods that exploit optical-field photoemission from plasmonic nanoantennas. These devices make for compact and integratable solid-state detectors operating at optical frequency that work in ambient conditions and require minute pulse energies (picojoule-level). Applications include frequency-comb stabilization, visible to near-infrared time-domain spectroscopy, compact tools for attosecond science and metrology and, due to the hig…
We describe Ti:Sapphire pumped optical parametric amplification of carrier-envelope phase stabilized few-cycle ($<10$fs) mid-infrared pulses in type I $β$-barium borate. Experimental measurements show a $\times3.5$ amplification factor (from 100$μ$J to 350$μ$J) of the octave spanning spectrum ($1.1-2.4$$μ$m) using a pump beam with 2.3mJ energy, 30fs duration and central wavelength of 800nm, corresponding to an energy extraction efficiency of $11\%$. Numerical simulations suggest potential amplification to 4.25mJ energy and temporal compression to a pulse duration of 7.3fs is possible with a pu…
High-brightness sources of coherent and few-cycle-duration light waveforms with spectral coverage from the UV to the THz would offer unprecedented versatility and opportunities for a spectacular range of applications from bio-chemical sensing, to time-resolved and nonlinear spectroscopy, to attosecond light-wave electronics. Combinations of various sources with frequency conversion and supercontinuum generation can provide relatively large spectral coverage, but many applications require much broader spectral range and low-jitter synchronization for time-domain measurements. Here, we present a…
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 $\textμ$m region and intra-pulse difference-frequency generation in the 4--5 $\textμ$m region. By engineering the quasi-phase-matched grating profiles, tunable, narrow-band MIR and broadband MIR spectra are both observed in this geometry. Final…
In supercontinuum generation, various propa- gation effects combine to produce a dramatic spec- tral broadening of intense ultrashort optical pulses with far reaching possibilities. Different applications place highly divergent and challenging demands on source characteristics such as spectral coverage from the ultraviolet (UV) across the visible (VIS) to the near-infrared (NIR), and into the mid-infrared (MIR). Shot-to-shot repeatability, high spectral energy density, an absence of complicated or non-deterministic pulse splitting are also essential for many applications. Here we present an "a…
We report on the development of a high-power mid-infrared frequency comb with 100 MHz repetition rate and 100 fs pulse duration. Difference frequency generation is realized between two branches derived from an Er:fiber comb, amplified separately in Yb:fiber and Er:fiber amplifiers. Average powers of 6.7 W and 14.9 W are generated in the 2.9 $μ$m idler and 1.6 $μ$m signal, respectively. With high average power, excellent beam quality, and passive carrier-envelope phase stabilization, this light source is a promising platform for generating broadband frequency combs in the far infrared, visible,…
We present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing…
Carrier envelope phase (CEP) stabilized 5 fs and 22 fs pulses of intense 800 nm light are used to probe the strong-field ionization dynamics of multielectron entities, xenon and carbon disulfide. We compare ion yields obtained with and without CEP-stabilization: with 8-cycle (22 fs) pulses, Xe$^{6+}$ yields are suppressed (relative to Xe$^+$ yields) by between 30% and 50%, depending on phase, reflecting the phase dependence of non-sequential ionization and its contribution to the formation of higher charge states. On the other hand, ion yields for Xe$^{q+}$ ($q$=2-4) with CEP-stablized pulses …
We have built a frequency chain which enables to measure the absolute frequency of a laser emitting in the 28-31 THz frequency range and stabilized onto a molecular absorption line. The set-up uses an optical frequency comb and an ultrastable 1.55 $μ$m frequency reference signal, transferred from LNE-SYRTE to LPL through an optical link. We are now progressing towards the stabilization of the mid-IR laser via the frequency comb and the extension of this technique to quantum cascade lasers. Such a development is very challenging for ultrahigh resolution molecular spectroscopy and fundamental te…
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 ($\mathbf{\lesssim}$15 fs, 100 pJ) from a near-infrared (NIR) 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--4.1 $μ$m region, while orientation-patterned gallium phosphide provides coverage across 7--11 $μ$m. Casca…
We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dep…
We describe a coherent mid-infrared continuum source with 700 cm-1 usable bandwidth, readily tuned within 600 - 2500 cm-1 (4 - 17 \mum) and thus covering much of the infrared "fingerprint" molecular vibration region. It is based on nonlinear frequency conversion in GaSe using a compact commercial 100-fs-pulsed Er fiber laser system providing two amplified near-infrared beams, one of them broadened by a nonlinear optical fiber. The resulting collimated mid-infrared continuum beam of 1 mW quasi-cw power represents a coherent infrared frequency comb with zero carrier-envelope phase, containing ab…
High resolution and fast detection of molecular vibrational absorption is important for organic synthesis, pharmaceutical process and environmental monitoring, and is enabled by mid-infrared (mid-IR) laser frequency combs via dual-comb spectroscopy. Here, we demonstrate a novel and highly simplified approach to broadband mid-IR dual-comb spectroscopy via supercontinuum generation, achieved using unprecedented nanophotonic dispersion engineering that allows for flat-envelope, ultra-broadband mid-IR comb spectra. The mid-IR dual-comb has an instantaneous bandwidth covering the functional group r…
We report a few-cycle, broadband, singly-resonant optical parametric oscillator (OPO) for the mid-infrared based on MgO-doped periodically-poled LiNbO3 (MgO:PPLN), synchronously pumped by a 20-fs Ti:sapphire laser. By using crystal interaction lengths as short as 250 um, and careful dispersion management of input pump pulses and the OPO resonator, near-transform-limited, few-cycle idler pulses tunable across the mid-infrared have been generated, with as few as 3.7 optical cycles at 2682 nm. The OPO can be continuously tuned over 2179-3732 nm by cavity delay tuning, providing up to 33 mW of out…
We present high-reflectivity substrate-transferred single-crystal GaAs/AlGaAs interference coatings at a center wavelength of 4.54 um with record-low excess optical loss below 10 parts per million. These high-performance mirrors are realized via a novel microfabrication process that differs significantly from the production of amorphous multilayers generated via physical vapor deposition processes. This new process enables reduced scatter loss due to the low surface and interfacial roughness, while low background doping in epitaxial growth ensures strongly reduced absorption. We report on a su…
