Many-wavelength interferometry with thousands of lasers for absolute distance measurement

We demonstrate a new technique for absolute distance measurement with a femtosecond frequency comb laser, based on unraveling the output of an interferometer to distinct comb modes with 1?GHz spacing. From the fringe patterns that are captured with a camera, a distance is derived by combining spectral and homodyne interferometry, exploiting about 9000 continuous wave lasers. This results in a measurement accuracy far within an optical fringe (λ/30), combined with a large range of nonambiguity (15?cm). Our technique merges multiwavelength interferometry and spectral interferometry, within a single scheme.     

Quantum-noise-limited optical frequency comb spectroscopy

We achieve a quantum-noise-limited absorption sensitivity of 1.7×10(-12) cm(-1) per spectral element at 400 s of acquisition time with cavity-enhanced frequency comb spectroscopy, the highest demonstrated for a comb-based technique. The system comprises a frequency comb locked to a high-finesse cavity and a fast-scanning Fourier transform spectrometer with an ultralow-noise autobalancing detector. Spectra with a signal-to-noise ratio above 1000 and a resolution of 380 MHz are acquired within a few seconds. The measured absorption line shapes are in excellent agreement with theoretical predictions.     

Octave-spanning frequency comb generation in a silicon nitride chip

We demonstrate a frequency comb spanning an octave via the parametric process of cascaded four-wave mixing in a monolithic, high-Q silicon nitride microring resonator. The comb is generated from a single-frequency pump laser at 1562?nm and spans 128?THz with a spacing of 226?GHz, which can be tuned slightly with the pump power. In addition, we investigate the RF amplitude noise characteristics of the parametric comb and find that the comb can operate in a low-noise state with a 30?dB reduction in noise as the pump frequency is tuned into the cavity resonance.     

脉冲升温纳秒时间分辨中红外光谱研究氨基酸重水溶液的分子间氢键

应用变温傅立叶变换红外光谱和脉冲升温纳秒时间分辨红外差谱研究了组氨酸和甘氨酸的重水溶液的羧基负离子的振动．结果表明不仅氨基酸分子之间形成氢键，而且氨基酸分子和溶剂分子之间也形成氢键．当温度升高时，羧基负离子在1600?1610 cm?1 附近的反对称伸缩振动发生蓝移，说明高温使氢键减弱．温度从10℃突然升高到20℃，组氨酸的时间分辨瞬态光谱出现两个漂白峰，一个在1604 cm?1，指认为形成氨基酸分子间氢键的羧基负离子的峰；另一个在1612 cm?1，指认为氨基酸分子和溶剂分子形成氢键的羧基负离子的峰．前     

飞秒光学频率梳高精度气体吸收光谱技术进展

飞秒光学频率梳以其频谱宽、脉宽窄、频率稳定度高等优点,对光学频率计量、绝对距离测量、高精度光谱测定产生重大影响。飞秒光学频率梳的时域特性和频域特性溯源至微波频率基准,使得高精度气体吸收光谱探测成为可能。飞秒光学频率梳光谱技术具有测量速度快、光谱灵敏度高、分辨率高、信噪比高等优点,因此加大对飞秒光学频率梳光谱技术的研究力度将更好地服务于环境保护、工业生产、生物医学、科学研究等各领域。飞秒光频梳高精度气体吸收光谱主要可分为光频梳腔衰荡光谱、光频梳腔增强光谱和双光频梳多外差光谱。其中,根据采集方式不同,光频梳腔增强光谱又可分为梳齿游标测量法、虚拟成像相位阵列测量法和傅里叶变换测量法。目前,国外已广泛开展相关研究,而国内仍处于起步阶段。本文综述了飞秒光学频率梳高精度气体吸收光谱探测的主要技术方法,展示了不同测量方法典型的实验方案,分析了各探测方法的优缺点,并追踪了主要研究小组的前沿成果。     

Cavity-enhanced direct frequency comb spectroscopy

Cavity-enhanced direct frequency comb spectroscopy combines broad spectral bandwidth, high spectral resolution, precise frequency calibration, and ultrahigh detection sensitivity, all in one experimental platform based on an optical frequency comb interacting with a high-finesse optical cavity. Precise control of the optical frequency comb allows highly efficient, coherent coupling of individual comb components with corresponding resonant modes of the high-finesse cavity. The long cavity lifetime dramatically enhances the effective interaction between the light field and intracavity matter, increasing the sensitivity for measurement of optical losses by a factor that is on the order of the cavity finesse. The use of low-dispersion mirrors permits almost the entire spectral bandwidth of the frequency comb to be employed for detection, covering a range of ～?10% of the actual optical frequency. The light transmitted from the cavity is spectrally resolved to provide a multitude of detection channels with spectral resolutions ranging from several gigahertz to hundreds of kilohertz. In this review we will discuss the principle of cavity-enhanced direct frequency comb spectroscopy and the various implementations of such systems. In particular, we discuss several types of UV, optical, and IR frequency comb sources and optical cavity designs that can be used for specific spectroscopic applications. We present several cavity-comb coupling methods to take advantage of the broad spectral bandwidth and narrow spectral components of a frequency comb. Finally, we present a series of experimental measurements on trace gas detections, human breath analysis, and characterization of cold molecular beams. These results demonstrate clearly that the wide bandwidth and ultrasensitive nature of the femtosecond enhancement cavity enables powerful real-time detection and identification of many molecular species in a massively parallel fashion.     

Kilohertz-resolution spectroscopy of cold atoms with an optical frequency comb

We have performed sub-Doppler spectroscopy on the narrow intercombination line of cold calcium atoms using the amplified output of a femtosecond laser frequency comb. Injection locking of a 657-nm diode laser with a femtosecond comb allows for two regimes of amplification, one in which many lines of the comb are amplified, and one where a single line is predominantly amplified. The output of the laser in both regimes was used to perform kilohertz-level spectroscopy. This experiment demonstrates the potential for high-resolution absolute-frequency spectroscopy over the entire spectrum of the frequency comb output using a single high-finesse optical reference cavity.     

Noise properties of an optical frequency comb from a SESAM-mode-locked 1.5-μm solid-state laser stabilized to the 10?13 level

We present a detailed investigation of the noise properties of an optical frequency comb generated from a femtosecond diode-pumped solid-state laser operating in the 1.5-??m spectral region. The stabilization of the passively mode-locked Er:Yb:glass laser oscillator, referred to as ERGO, is achieved using pump power modulation for the control of the carrier envelope offset (CEO) frequency and by adjusting the laser cavity length for the control of the repetition rate. The stability and the noise of the ERGO comb are characterized in free-running and in phase-locked operation by measuring the noise properties of the CEO, of the repetition rate, and of a comb line at 1558?nm. The comb line is analyzed from the heterodyne beat signal with a cavity-stabilized ultra-narrow-linewidth laser using a frequency discriminator. Two different schemes to stabilize the comb to a radio-frequency (RF) reference are compared. The comb properties (phase noise, frequency stability) are limited in both cases by the RF oscillator used to stabilize the repetition rate, while the contribution of the CEO is negligible at all Fourier frequencies, as a consequence of the low-noise characteristics of the CEO-beat. A?linewidth of ??150?kHz and a fractional frequency instability of 4.2×10^?13 at 1?s are obtained for an optical comb line at 1558?nm. Improved performance is obtained by stabilizing the comb to an optical reference, which is a cavity-stabilized ultra-narrow linewidth laser at 1558?nm. The fractional frequency stability of 8×10^?14 at 1?s, measured in preliminary experiments, is limited by the reference oscillator used in the frequency comparison.     

Single-pass high-harmonic generation at 20.8 MHz repetition rate

We report on single-pass high-harmonic generation (HHG) with amplified driving laser pulses at a repetition rate of 20.8?MHz. An Yb:YAG Innoslab amplifier system provides 35?fs pulses with 20?W average power at 1030?nm after external pulse compression. Following tight focusing into a xenon gas jet, we observe the generation of high-harmonic radiation of up to the seventeenth order. Our results show that state-of-the-art amplifier systems have become a promising alternative to cavity-assisted HHG for applications that require high repetition rates, such as frequency comb spectroscopy in the extreme UV.     

A direct frequency comb for two-photon transition spectroscopy in a cesium vapor

A phase-stabilized femtosecond frequency comb is used to measure high-resolution spectra of two-photon transition 62S1/2-62P1/2,3/2-82S1/2 in a cesium vapor.The broadband laser output from a femtosecond frequency comb is split into counter-propagating parts,shaped in an original way,and focused into a room-temperature cesium vapor.We obtain high-resolution two-photon spectroscopy by scanning the repetition rate of femtosecond frequency comb,and through absolute frequency measurements.     

Passively mode-locked 10 GHz femtosecond Ti:sapphire laser

We report a mode-locked Ti:sapphire femtosecond laser emitting 42 fs pulses at a 10 GHz repetition rate. When operated with a spectrally integrated average power greater than 1 W, the associated femtosecond laser frequency comb contains approximately 500 modes, each with power exceeding 1 mW. Spectral broadening in nonlinear microstructured fiber yields comb elements with individual powers greater than 1 nW over approximately 250 nm of spectral bandwidth. The modes of the emitted comb are resolved and imaged with a simple grating spectrometer and digital camera. Combined with absorption spectroscopy of rubidium vapor, this approach permits identification of the mode index and measurement of the carrier envelope offset frequency of the comb.     

Bandwidth scaling and spectral flatness enhancement of optical frequency combs from phase-modulated continuous-wave lasers using cascaded four-wave mixing

We introduce a new cascaded four-wave mixing technique that scales up the bandwidth of frequency combs generated by phase modulation of a continuous-wave (CW) laser while simultaneously enhancing the spectral flatness. As a result, we demonstrate a 10?GHz frequency comb with over 100?lines in a 10?dB bandwidth in which a record 75?lines are within a flatness of 1?dB. The cascaded four-wave mixing process increases the bandwidth of the initial comb generated by the modulation of a CW laser by a factor of five. The broadband comb has approximately quadratic spectral phase, which is compensated upon propagation in single-mode fiber, resulting in a 10?GHz train of 940?fs pulses.     

Ultrafast optical frequency comb synthesizer and analyzer

We propose an ultrafast optical arbitrary waveform synthesizing/analyzing technique demonstrated with 2 Tbit/s waveforms. An ultrafast waveform was generated by manipulating the amplitude and phase of a 400?GHz optical frequency comb using a newly developed colorless optical synthesizer. The 400?GHz optical frequency comb was generated from a 25?GHz optical frequency comb using a colorless arrayed waveguide grating. This waveform was then analyzed on the frequency axis using a custom heterodyne-detection technique based on the dual-heterodyne mixing method. The phase and amplitude spectra can be observed in parallel using another optical frequency comb as a reference combined with an arrayed waveguide grating. This optical system, named the ultrafast optical frequency comb synthesizer and analyzer, can synthesize and analyze an arbitrary waveform in the THz frequency region.     

High-resolution spectroscopy using interleaved 100 GHz optical frequency comb scanned by phase modulator

A high-resolution spectroscopy technique is proposed with an optical phase modulator combined with an interleaved optical frequency comb. The optical phase modulator and a frequency-locked laser light guarantee a spectral resolution less than 1 MHz on an absolute frequency axis. A wide measurement frequency range was realized using a 25 GHz optical frequency comb lying over a 4 THz frequency region. An extraction of single tooth intensity from the comb was realized by a heterodyne technique with a frequency-tunable laser used as a local oscillator. Also, the 25 GHz optical frequency comb was interleaved to generate four 100-GHz combs for removing the crosstalk from the 25 GHz neighboring sidebands in the teeth. This proposed spectroscopy technique was experimentally demonstrated with a resonator of less than 1 MHz linewidth and a H¹³C¹⁴N gas cell. Thus, a measurement frequency range higher than 4 THz (1530 nm-1560 nm) was confirmed with an effective spectral resolution 100 kHz order. In addition, the characteristics of the proposed system were compared with those of the previous system with a single-sideband (SSB) optical modulator.     

Einstein Lecture – Passion for precision

Optical frequency combs from mode‐locked femtosecond lasers have link optical and microwave frequencies in a single step, and they provide the long missing clockwork for optical atomic clocks. By extending the limits of time and frequency metrology, they enable new tests of fundamental physics laws. Precise comparisons of optical resonance frequencies of atomic hydrogen and other atoms with the microwave frequency of a cesium atomic clock are establishing sensitive limits for possible slow variations of fundamental constants. Optical high harmonic generation is extending frequency comb techniques into the extreme ultraviolet, opening a new spectral territory to precision laser spectroscopy. Frequency comb techniques are also providing a key to attosecond science by offering control of the electric field of ultrafast laser pulses. In our laboratories at Stanford and Garching, the development of new instruments and techniques for precision laser spectroscopy has long been motivated by the goal of ever higher resolution and measurement accuracy in optical spectroscopy of the simple hydrogen atom which permits unique confrontations between experiment and fundamental theory. This lecture recounts these adventures and the evolution of laser frequency comb techniques from my personal perspective.     

Fiber-based optical frequency comb at 3.3 μm for broadband spectroscopy of hydrocarbons [Invited]

A 125 MHz fiber-based frequency comb source in the mid-infrared wavelength region is presented. The source is based on difference frequency generation from a polarization-maintaining Er-doped fiber pump laser and covers a spectrum between2900 cm~(-1) and 3400 cm~(-1) with a simultaneous bandwidth of 170 cm~(-1) and an average output power up to 70 m W. The source is equipped with actuators and active feedback loops, ensuring long-term stability of the repetition rate, output power, and spectral envelope. An absorption spectrum of ethane and methane was measured using a Fourier transform spectrometer to verify the applicability of the mid-infrared comb to multispecies detection. The robustness and good long-and short-term stability of the source make it suitable for optical frequency comb spectroscopy of hydrocarbons.     

Widely tunable THz synthesizer

The generation of cw-THz radiation by photomixing is particularly suited to the high resolution spectroscopy of gases; nevertheless, until recently, it has suffered from a lack of frequency metrology. Frequency combs are a powerful tool that can transfer microwave frequency standards to optical frequencies and a single comb has permitted accurate (10⁻⁸) THz frequency synthesis with a limited tuning range. A THz synthesizer composed of three extended cavity laser diodes phase locked to a frequency comb has been constructed and its utility for high resolution gas phase spectroscopy demonstrated. The third laser diode allows a larger tuning range of up to 300 MHz to be achieved without the need for large frequency excursions, while the frequency comb provides a versatile link to be established from any traceable microwave frequency standard. The use of a single frequency comb as a reference for all of the cw-lasers eliminates the dependency of synthesized frequency on the carrier envelope offset frequency. This greatly simplifies the frequency comb stabilization requirements and leads to a reduced instrument complexity.     

A rapid,spatially dispersive frequency comb spectrograph aimed at gas phase chemical reaction kinetics

This New Views article will highlight some recent advances in high sensitivity gas detection using direct infrared absorption frequency comb laser spectroscopy, with a focus on frequency comb use in chemical reaction kinetics and our own contribution to this field. Our recently implemented detection technique uses a combination of a 12.9?GHz free spectral range virtually imaged phased array and diffraction grating to spatially disperse the mid-infrared frequency comb onto a camera. Individual frequencies or ‘comb teeth’ of a 250?MHz repetition-rate frequency comb are able to be resolved. High molecular sensitivity is achieved by increasing the interaction path length using a Herriott multipass cell. High spectral resolution, broadband spectral coverage, and high molecular sensitivity are all achieved on an adjustable 1–50 µs timescale, making this frequency comb apparatus ideal for measuring chemical reaction kinetics where multiple absorbing species can be monitored simultaneously. This New Views article will also discuss some of the challenges and decisions that chemists might face in implementing this advanced physics technology in their own laboratory.

Spatially dispersed 250 MHz mid-infrared frequency comb laser, with absorption of some frequencies by a dilute sample of methane.     

Velocity selective optical pumping of Rb hyperfine lines induced by a train of femtosecond pulses

We present direct observation of the velocity-selective optical pumping of the Rb ground state hyperfine levels induced by 5S(1/2) --> 5P(1/2) femtosecond pulse-train excitation. A modified direct frequency comb spectroscopy based on the fixed frequency comb and a weak cw scanning probe laser was developed. The femtosecond pulse-train excitation of a Doppler-broadened Rb four-level atomic vapor is investigated theoretically in the context of the density matrix formalism and the results are compared with the experiment.