Control of four-level quantum coherence via discrete spectral shaping of an optical frequency comb.

We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. Finally, the pulse shape is optimized resulting in a 256% increase in the two-photon transition rate by forcing constructive interference between the mode pairs detuned from an intermediate resonance.

Precise control of molecular dynamics with a femtosecond frequency comb.

We present a general and highly efficient scheme for performing narrow-band Raman transitions between molecular vibrational levels using a coherent train of weak pump-dump pairs of shaped ultrashort pulses. The use of weak pulses permits an analytic description within the framework of coherent control in the perturbative regime, while coherent accumulation of many pulse pairs enables near unity transfer efficiency with a high spectral selectivity, thus forming a powerful combination of pump-dump control schemes and the precision of the frequency comb. Simulations verify the feasibility and robustness of this concept, with the aim to form deeply bound, ultracold molecules.

High resolution atomic coherent control via spectral phase manipulation of an optical frequency comb.

We demonstrate high resolution coherent control of cold atomic rubidium utilizing spectral phase manipulation of a femtosecond optical frequency comb. Transient coherent accumulation is directly manifested by the enhancement of signal amplitude and spectral resolution via the pulse number. The combination of frequency comb technology and spectral phase manipulation enables coherent control techniques to enter a new regime with natural linewidth resolution.

Tapered semiconductor amplifiers for optical frequency combs in the near infrared.

A tapered semiconductor amplifier is injection seeded by a femtosecond optical frequency comb at 780 nm from a mode-locked Ti:sapphire laser. Energy gains of more than 17 dB(12 dB) are obtained for 1 mW(20 mW) of average input power when the input pulses are stretched into the picosecond range. A spectral window of supercontinuum light generated in a photonic fiber has also been amplified. Interferometric measurements show sub-Hertz linewidths for a heterodyne beat between the input and amplified comb components, yielding no detectable phase-noise degradation under amplification. These amplifiers can be used to boost the infrared power in f-to-2f interferometers used to determine the carrier-to-envelope offset frequency, with clear advantages for stabilization of octave-spanning femtosecond lasers and other supercontinuum light sources.

Direct frequency comb measurements of absolute optical frequencies and population transfer dynamics.

A phase-stabilized femtosecond laser comb is directly used for high-resolution spectroscopy and absolute optical frequency measurements of one- and two-photon transitions in laser-cooled 87Rb atoms. Absolute atomic transition frequencies, such as the 5S1/2 F=2-->7S1/2 F"=2 two-photon resonance measured at 788,794 768,921 (44) kHz, are determined without a priori knowledge about their values. Detailed dynamics of population transfer driven by a sequence of pulses are uncovered and taken into account for the measurement of the 5P states via resonantly enhanced two-photon transitions.

United time-frequency spectroscopy for dynamics and global structure.

Ultrashort laser pulses have thus far been used in two distinct modes. In the time domain, the pulses have allowed probing and manipulation of dynamics on a subpicosecond time scale. More recently, phase stabilization has produced optical frequency combs with absolute frequency reference across a broad bandwidth. Here we combine these two applications in a spectroscopic study of rubidium atoms. A wide-bandwidth, phase-stabilized femtosecond laser is used to monitor the real-time dynamic evolution of population transfer. Coherent pulse accumulation and quantum interference effects are observed and well modeled by theory. At the same time, the narrow linewidth of individual comb lines permits a precise and efficient determination of the global energy-level structure, providing a direct connection among the optical, terahertz, and radio-frequency domains. The mechanical action of the optical frequency comb on the atomic sample is explored and controlled, leading to precision spectroscopy with an appreciable reduction in systematic errors.