Christoph Gohle

Time-domain mid-infrared frequency-comb spectrometer

A novel type of Fourier-transform infrared spectrometer (FTIR) is demonstrated. It is based on two Ti:sapphire lasers emitting femtosecond pulse trains with slightly different repetition frequencies. Two mid-infrared beams-derived from those lasers by rectification in GaSe-are superimposed upon a detector to produce purely time-domain interferograms that encode the infrared spectrum. The advantages of this spectrometer compared with the common FTIR include ease of operation (no moving parts), speed of acquisition (100 micros demonstrated), and not-yet-shown collimated long-distance propagation, diffraction-limited microscopic probing, and electronically controllable chemometric factoring. Extending time-domain frequency-comb spectroscopy to lower (terahertz) or higher (visible, ultraviolet) frequencies should be feasible.

A frequency comb in the extreme ultraviolet

Since 1998, the interaction of precision spectroscopy and ultrafast laser science has led to several notable accomplishments. Femtosecond laser optical frequency ‘combs’ (evenly spaced spectral lines) have revolutionized the measurement of optical frequencies and enabled optical atomic clocks. The same comb techniques have been used to control the waveform of ultrafast laser pulses, which permitted the generation of single attosecond pulses, and have been used in a recently demonstrated ‘oscilloscope’ for light waves. Here we demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science. We have generated coherent extreme ultraviolet radiation at a repetition frequency of more than 100 MHz, a 1,000-fold improvement over previous experiments. At such a repetition rate, the mode spacing of the frequency comb, which is expected to survive the high harmonic generation process, is large enough for high resolution spectroscopy. Additionally, there may be many other applications of such a quasi-continuous compact and coherent extreme ultraviolet source, including extreme ultraviolet holography, microscopy, nanolithography and X-ray atomic clocks.

Frequency Comb Vernier Spectroscopy for Broadband, High-Resolution, High-Sensitivity Absorption and Dispersion Spectra

A femtosecond frequency comb provides a vast number of equidistantly spaced narrow band laser modes that can be simultaneously tuned and frequency calibrated with 15 digits accuracy. Our Vernier spectrometer utilizes all of theses modes in a massively parallel manner to rapidly record both absorption and dispersion spectra with a sensitivity that is provided by a high finesse broad band optical resonator and a resolution that is only limited by the frequency comb line width while keeping the required setup simple. PACS numbers: 42.62.Fi, 42.62.Eh, 42.30.Rx, 42.25.Bs, 42.30.Ms. Electronic address: ctg@mpq.mpg.de Now at Physikalisch Technische Bundesanstalt, Braunschweig, Germany

Monolithic carrier-envelope phase-stabilization scheme

A new scheme for stabilizing the carrier-envelope (CE) phase of a few-cycle laser pulse train is demonstrated. Self-phase modulation and difference-frequency generation in a single periodically poled lithium niobate crystal that transmits the main laser beam allows CE phase locking directly in the usable output. The monolithic scheme obviates the need for splitting off a fraction of the laser output for CE phase control, coupling into microstructured fiber, and separation and recombination of spectral components. As a consequence, the output yields 6-fs, 800-nm pulses with an unprecedented degree of short- and long-term reproducibility of the electric field waveform.

Optical clockwork with an offset-free difference-frequency comb: accuracy of sum- and difference-frequency generation

We demonstrate a simple optical clockwork mechanism based on the broadened frequency comb of a femtosecond laser and on difference-frequency generation (DFG) in a nonlinear crystal. The DFG comb possesses a vanishing carrier envelope offset frequency that permits the construction of a simple and thus potentially more stable optical clockwork. In addition it offers the possibility of extending the frequency comb into the infrared spectral region. The overall accuracy and stability of the DFG comb relative to the initial frequency comb were measured to be 6.6 x 10(-21) and 10(-18) tau(-1), respectively, where tau is the averaging time in seconds. Assuming that sum- and difference-frequency generation are independent processes, our measurements suggest a <10(-20) accuracy for them.

Extreme Ultraviolet Frequency Comb Metrology

The remarkable precision of frequency-comb (FC) lasers is transferred to the extreme ultraviolet (XUV, wavelengths shorter than 100 nm), a frequency region previously not accessible to these devices. A frequency comb at XUV wavelengths near 51 nm is generated by amplification and coherent up-conversion of a pair of pulses originating from a near-infrared femtosecond FC laser. The phase coherence of the source in the XUV is demonstrated using helium atoms as a ruler and phase detector. Signals in the form of stable Ramsey-like fringes with high contrast are observed when the FC laser is scanned over P states of helium, from which the absolute transition frequency in the XUV can be extracted. This procedure yields a (4)He ionization energy at h×5 945 204 212(6)  MHz, improved by nearly an order of magnitude in accuracy, thus challenging QED calculations of this two-electron system.

Attosecond control of optical waveforms

A new, monolithic scheme for stabilizing the phase between the carrier wave and the envelope (CE phase) in a train of few-cycle laser pulses is demonstrated. Self-phase modulation and second-harmonic generation or difference-frequency generation in a single periodically poled lithium niobate crystal, that transmits the main laser beam, allows for the CE-phase locking directly in the usable output. The monolithic scheme obviates the need for splitting off a fraction of the laser output for CE-phase control, coupling into microstructured fibre, as well as separation and recombination of spectral components. As a result, the CE-phase error integrated over the spectral range of 0.2 mHz–35 MHz is as small as 0.016 × 2π rad. This implies that the phase of the field oscillations (λ ~ 830 nm) with respect to the pulse peak is locked to within 44 attoseconds, resulting in optical waveform control with subhundred attosecond fidelity for the first time.

Precision spectroscopy of hydrogen and femtosecond laser frequency combs

Precision spectroscopy of the simple hydrogen atom has inspired dramatic advances in optical frequency metrology: femtosecond laser optical frequency comb synthesizers have revolutionized the precise measurement of optical frequencies, and they provide a reliable clock mechanism for optical atomic clocks. Precision spectroscopy of the hydrogen 1S–2S two-photon resonance has reached an accuracy of 1.4 parts in 1014, and considerable future improvements are envisioned. Such laboratory experiments are setting new limits for possible slow variations of the fine structure constant α and the magnetic moment of the caesium nucleus μCs in units of the Bohr magneton μB.

Complete characterization of a broadband high-finesse cavity using an optical frequency comb

We demonstrate a new method to simultaneously measure spectrally resolved dispersion and losses (finesse) of a passive optical cavity over the entire bandwidth of an optical frequency comb. To this end, we record and analyze the spectral Moiré pattern between the perfectly equidistant frequency comb emitted from a Ti:Sapphire laser and the longitudinal modes of the passive cavity as a function of the lasers carrier-envelope-offset phase slippage (ø)CE. In the group-delay dispersion measurement of additionally introduced optical elements we verify a 2fs(2) accuracy in a 2THz resolution bandwidth and find good agreement of the measured performance and the target design of a high reflectance dielectric mirror. The sensitivity of the method is essentially equivalent to a cavity ring down technique allowing us also to readily observe signatures of atmospheric gas species.

Frequency metrology on the 4s(2)S(1/2)-4p(2)P(1/2) transition in Ca-40(+) for a comparison with quasar data

High accuracy frequency metrology on the 4s S-2(1/2)-4p P-2(1/2) transition in calcium ions is performed using laser cooled and crystallized ions in a linear Paul trap. Calibration is performed with a frequency comb laser, resulting in a transition frequency of f = 755 222 766.2 (1.7) MHz. The accuracy presents an improvement of more than one order of magnitude, and will facilitate a comparison with quasar data in a search for a possible change of the fine structure constant on a cosmological time scale.