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J. L. Carini

Publications and source records attributed to J. L. Carini.

12 recordsLinked to original sources

Directional Quantum-Controlled Chemistry: Generating Aligned Ultracold Molecules via Photoassociation

Photoassociation of ultracold atoms is shown to lead to alignment of the product molecules along the excitation laser polarization axis. We theoretically investigate pulsed photoassociation of $^{87}Rb$ atoms into a specific weakly-bound level of the a $^3Σ_u^+$ metastable electronic state and find both stationary and time-dependent field-free alignment. Although a transform-limited pulse yields significant alignment, a frequency-chirped pulse dramatically enhances the molecular formation rate at the cost of a slight decrease in the alignment. Employing multiple pulses synchronized with the vibrational and rotational periods leads to coherent enhancement of both population and alignment of the target state.

quant-ph

High-Resolution Spectroscopy of {R}ydberg Molecular States of $^{85}${R}b$_2$ Near the $5s+7p$ Asymptote

Rydberg molecules, often exemplified by long-range "trilobite" molecules, are a subject of much recent interest at high principal quantum number $n$. States that use the same bonding mechanism can exist at much lower $n$ and less-extreme internuclear separations that are still quite long range. We use a high-resolution pulsed amplifier to study previously-detected transitions to a low-$n$ Rydberg molecular state near the $5s+7p$ asymptote in $^{85}$Rb$_2$. The observed line structure is modeled using precise ground-state positions and a lower bound of $τ> 1.1 \times 10^{-9}$ s is set on the excited-state autoionization lifetime.

physics.atom-ph

Short-range photoassociation from the inner wall of the lowest triplet potential of $^{85}$Rb$_2$

Ultracold photoassociation is typically performed at large internuclear separations, where the scattering wavefunction amplitude is large and Franck-Condon overlap is maximized. Recently, work by this group and others on alkali-metal diatomics has shown that photoassociation can efficiently form molecules at short internuclear distance in both homonuclear and heteronuclear dimers. We propose that this short-range photoassociation is due to excitation near the wavefunction amplitude maximum at the inner wall of the lowest triplet potential. We show that Franck-Condon factors from the highest-energy bound state can almost precisely reproduce Franck-Condon factors from a low-energy scattering state, and that both calculations match experimental data from the near-zero positive-energy scattering state with reasonable accuracy. We also show that the corresponding photoassociation from the inner wall of the ground-state singlet potential at much shorter internuclear distance is weaker and undetectable under our current experimental conditions. We predict from Franck-Condon factors that the strongest of these weaker short-range photoassociation transitions are one order of magnitude below our current sensitivity.

physics.atom-ph

Efficient Formation of Ultracold Molecules with Chirped Nanosecond Pulses

We describe experiments and associated quantum simulations involving the production of ultracold $^{87}$Rb$_{2}$ molecules with nanosecond pulses of frequency-chirped light. With appropriate chirp parameters, the formation is dominated by coherent processes. For a positive chirp, excited molecules are produced by photoassociation early in the chirp, then transferred into high vibrational levels of the lowest triplet state by stimulated emission later in the chirp. Generally good agreement is seen between the data and the simulations. Shaping of the chirp can lead to a significant enhancement of the formation rate. Further improvements using higher intensities and different intermediate states are predicted.

physics.atom-ph

Enhancement of Ultracold Molecule Formation Using Shaped Nanosecond Frequency Chirps

We demonstrate that judicious shaping of a nanosecond-time-scale frequency chirp can dramatically enhance the formation rate of ultracold $^{87}$Rb$_{2}$ molecules. Starting with ultracold $^{87}$Rb atoms, we apply pulses of frequency-chirped light to first photoassociate the atoms into excited molecules and then, later in the chirp, de-excite these molecules into a high vibrational level of the lowest triplet state, $a \, ^{3}Σ_{u}^{+}$. The enhancing chirp shape passes through the absorption and stimulated emission transitions relatively slowly, thus increasing their adiabaticity, but jumps quickly between them to minimize the effects of spontaneous emission. Comparisons with quantum simulations for various chirp shapes support this enhancement mechanism.

physics.atom-ph

Production of Ultracold Molecules with Chirped Nanosecond Pulses: Evidence for Coherent Effects

We use frequency-chirped light on the nanosecond time scale to produce ultracold $^{87}$Rb$_{2}$ molecules in the lowest triplet state via the process of photoassociation. Comparing to quantum simulations of the molecular formation, we conclude that coherent stimulated emission plays an important role and is primarily responsible for the significant difference observed between positive and negative chirps.

physics.atom-ph

Coherent control of ultracold 85Rb trap-loss collisions with nonlinearly frequency-chirped light

We present results on coherent control of ultracold trap-loss collisions using 40 ns pulses of nonlinearly frequency-chirped light. The chirps, either positive or negative, sweep ~1 GHz in 100 ns and are centered at various detunings below the D2 line of 85Rb. At each center detuning, we compare the collisional rate constant beta for chirps that are linear in time, concave-down and concave-up. For positive chirps, we find that beta generally depends very little on the shape of the chirp. For negative chirps, however, we find that beta can be enhanced by up to 50(20)% for the case of the concave-down shape. This occurs at detunings where the evolution of the wavepacket is expected to be coherent. An enhancement at these detunings is also seen in quantum mechanical simulations of the collisional process.

physics.atom-ph

Creation of arbitrary spectra with an electro-optic modulator

We use a waveguide-based electro-optic phase modulator, driven by a nanosecond-timescale arbitrary waveform generator, to produce an optical spectrum with an arbitrary pattern of sidebands. A programmed sequence of linear voltage ramps, with various slopes, is applied to the modulator. The resulting phase ramps give rise to sidebands whose frequency offsets relative to the carrier are equal to the slopes of the corresponding linear phase ramps. This extension of the serrodyne technique provides multi-line spectra with sideband spacings in the 100 MHz range.

physics.atom-ph

Characterization and Compensation of the Residual Chirp in a Mach-Zehnder-Type Electro-Optical Intensity Modulator

We utilize various techniques to characterize the residual phase modulation of a fiber-based Mach-Zehnder electro-optical intensity modulator. A heterodyne technique is used to directly measure the phase change due to a given change in intensity, thereby determining the chirp parameter of the device. This chirp parameter is also measured by examining the ratio of sidebands for sinusoidal amplitude modulation. Finally, the frequency chirp caused by an intensity pulse on the nanosecond time scale is measured via the heterodyne signal. We show that this chirp can be largely compensated with a separate phase modulator. The various measurements of the chirp parameter are in reasonable agreement.

physics.atom-ph

Coherent Control of Ultracold Collisions with Chirped Light: Direction Matters

We demonstrate the ability to coherently control ultracold atomic Rb collisions using frequency-chirped light on the nanosecond time scale. For certain center frequencies of the chirp, the rate of inelastic trap-loss collisions induced by negatively chirped light is dramatically suppressed compared to the case of a positive chirp. We attribute this to a fundamental asymmetry in the system: an excited wavepacket always moves inward on the attractive molecular potential. For a positive chirp, the resonance condition moves outward in time, while for a negative chirp, it moves inward, in the same direction as the excited wavepacket; this allows multiple interactions between the wavepacket and the light, enabling the wavepacket to be returned coherently to the ground state. Classical and quantum calculations support this interpretation.

physics.atom-ph

Generation of Arbitrary Frequency Chirps with a Fiber-Based Phase Modulator and Self-Injection-Locked Diode Laser

We present a novel technique for producing pulses of laser light whose frequency is arbitrarily chirped. The output from a diode laser is sent through a fiber-optical delay line containing a fiber-based electro-optical phase modulator. Upon emerging from the fiber, the phase-modulated pulse is used to injection-lock the laser and the process is repeated. Large phase modulations are realized by multiple passes through the loop while the high optical power is maintained by self-injection-locking after each pass. Arbitrary chirps are produced by driving the modulator with an arbitrary waveform generator.

physics.atom-ph

Probing Ultracold Collisional Dynamics with Frequency-Chirped Pulses

We report on the dynamics of ultracold collisions induced by near-resonant frequency-chirped light. A series of identical chirped pulses, separated by a variable delay, is applied to an ultracold sample of 85Rb, and the rate of inelastic trap-loss collisions is measured. For small detunings of the chirped light below the atomic resonance, we observe that the rate of collisions induced by a given pulse can be increased by the presence of an earlier pulse. We attribute this to the enhancement of short-range collisional flux by the long-range excitation of atom pairs to an attractive molecular potential. For larger detunings and short delays, we find that a leading pulse can suppress the rate of collisions caused by a following pulse. This is due to a depletion of short-range atom pairs by the earlier pulse. Comparison of our data to classical Monte-Carlo simulations of the collisions yields reasonable agreement.

physics.atom-ph