Driving rotational transitions in molecules on a chip.

Polar molecules in selected quantum states can be guided, decelerated, and trapped using electric fields created by microstructured electrodes on a chip. Herein we explore how transitions between two of these quantum states can be induced while the molecules are on the chip. We use CO (a(3) Π(1) , v=0) molecules, prepared in the J=1 rotational level, and induce the J=2←J=1 rotational transition with narrow-band sub-THz (mm-wave) radiation. First, the mm-wave source is characterized using CO molecules in a freely propagating molecular beam, and both Rabi cycling and rapid adiabatic passage are examined. Then we demonstrate that the mm-wave radiation can be coupled to CO molecules that are less than 50 µm above the chip. Finally, CO molecules are guided in the J=1 level to the center of the chip where they are pumped to the J=2 level, recaptured, and guided off the chip.

Tunable frequency-controlled isolated attosecond pulses characterized by either 750 nm or 400 nm wavelength streak fields.

A compact and robust Mach-Zehnder type interferometer coupled with the double optical gating technique provides tunable isolated attosecond pulses and streak field detection with fields centered at either 750 nm or 400 nm. Isolated attosecond pulses produced at 45 eV (with measured pulse duration of 114 ± 4 as) and 20 eV (with measured pulse duration of 395 ± 6 as) are temporally characterized with a 750 nm wavelength streak field. In addition, an isolated 118 ± 10 as pulse at 45 eV is measured with a 400 nm wavelength streak field. The interferometer design used herein provides broad flexibility for attosecond streak experiments, allowing pump and probe pulses to be specified independently. This capability is important for studying selected electronic transitions in atoms and molecules.

Measurement and optimization of isolated attosecond pulse contrast.

An experimental method is presented to experimentally measure and control the carrier-envelope-phase (CEP)-dependent pulse-energy contrast of isolated attosecond pulses. By scanning the CEP and measuring the photoelectron spectrum produced by the combined action of the attosecond pulses and the high-harmonic driving laser pulses at zero relative time delay, one can extract the pulse-energy ratio between the main attosecond pulse and its neighboring satellite pulses arriving in preceding or subsequent half-cycles of the driver pulse. Moreover, this method allows fast and efficient in situ retrieval of the optimal CEP for high-contrast isolated attosecond pulse generation.

Generating coherent broadband continuum soft-x-ray radiation by attosecond ionization gating.

The current paradigm of isolated attosecond pulse production requires a few-cycle pulse as the driver for high-harmonic generation that has a cosine-like electric field stabilized with respect to the peak of the pulse envelope. Here, we present simulations and experimental evidence that the production of high-harmonic light can be restricted to one or a few cycles on the leading edge of a laser pulse by a gating mechanism that employs time-dependent ionization of the conversion medium. This scheme enables the generation of broadband and tunable attosecond pulses. Instead of fixing the carrier-envelope phase to produce a cosine driver pulse, the phase becomes a control parameter for the center frequency of the attosecond pulse. A method to assess the multiplicity of attosecond pulses in the pulse train is also presented. The results of our study suggest an avenue towards relaxing the requirement of few-cycle pulses for isolated attosecond pulse generation.

Heterodyne mixing of laser fields for temporal gating of high-order harmonic generation.

The concept of heterodyne mixing of laser fields is theoretically applied to the process of high-harmonic generation to enhance and modulate the kinetic energy of the active electron on subcycle time scales. A very small amount of intensity in the heterodyne field creates a significant modification of the electron kinetic energy, due to its amplification by the strong fundamental field in the kinetic-energy term, in which the heterodyne mixing occurs. Quantum calculations are carried out to verify the predictions of the classical results, demonstrating very good qualitative and quantitative agreement. Applications of the heterodyne-mixing concept are the extension of the harmonic cutoff to higher photon energies and the temporal gating of attosecond pulse production.

Circular phase mask for control and stabilization of single optical filaments.

We experimentally demonstrate an efficient way to control and stabilize single optical filaments initiated by ultrashort laser pulses in a rare gas medium. This is done by the application of a stationary two-dimensional phase mask to the laser beam prior to focusing. Simple circular phase-step patterns of a given radius and relative phase are sufficient to stabilize the pointing of the filament output and to optimize the spectral bandwidth of the light without any resulting loss of input laser power.

Single attosecond pulse generation in the multicycle-driver regime by adding a weak second-harmonic field.

We present a method of producing single attosecond pulses by high-harmonic generation with multicycle driver laser pulses. This can be achieved by tailoring the driving pulse so that attosecond pulses are produced only every full cycle of the oscillating laser field rather than every half-cycle. It is shown by classical and quantum-mechanical model calculations that even a minor addition (1%) of phase-locked second-harmonic light to the 800 nm fundamental driver pulse for high-harmonic generation leads to a major (15%) difference in the maximum kinetic energies of the recombining electrons in adjacent half-cycles.

Coherent Raman spectra of the nu1 mode of carbon suboxide.

High-resolution (0.001 cm(-1)) coherent anti-Stokes Raman spectroscopy (CARS) has been used to study the nu1 symmetric CO stretching mode of the quasi-linear molecule carbon suboxide, C3O2. Q-branch transitions are seen that originate from the ground state and from thermally populated levels of the nu7 CCC bending mode, which is of unusually low frequency. The intensity variation of the Q-branch features on cooling to about 120 K in a jet expansion requires the reversal of the order of assignment given in a previous Raman study at low resolution. The identification of the nu1 sigma(g)+ <-- sigma(g)+ transition from the ground state is confirmed by the absence of J(odd) Q-branch lines in the resolved CARS spectrum. Analysis of this band in terms of a quasi-linear model gives a good fit to the observed transitions and leads to vibrational-rotational parameters (in cm(-1)) of nu1 = 2199.9773(12) and (B' - B'') = -2.044(6) x 10(-4). Other transitions originating from higher nu7 levels occur at only slightly lower wavenumber values and permit the calculation of the double minimum potential in the Q7 bending coordinate. The results indicate that the ground-state barrier to linearity (21.5 cm(-1)) increases by only 0.6 cm(-1) when the CO symmetric stretch is excited.