Probing molecular potentials with an optical centrifuge.

We use an optical centrifuge to excite coherent rotational wave packets in N2O, OCS, and CS2 molecules with rotational quantum numbers reaching up to J≈465, 690, and 1186, respectively. Time-resolved rotational spectroscopy at such ultra-high levels of rotational excitation can be used as a sensitive tool to probe the molecular potential energy surface at internuclear distances far from their equilibrium values. Significant bond stretching in the centrifuged molecules results in the growing period of the rotational revivals, which are experimentally detected using coherent Raman scattering. We measure the revival period as a function of the centrifuge-induced rotational frequency and compare it with the numerical calculations based on the known Morse-cosine potentials.

Ultrafast Magnetization of a Dense Molecular Gas with an Optical Centrifuge.

Strong laser-induced magnetization of oxygen gas at room temperature and atmospheric pressure is achieved experimentally on the subnanosecond time scale. The method is based on controlling the electronic spin of paramagnetic molecules by means of manipulating their rotation with an optical centrifuge. Spin-rotational coupling results in a high degree of spin polarization on the order of one Bohr magneton per centrifuged molecule. Owing to the nonresonant interaction with the laser pulses, the demonstrated technique is applicable to a broad class of paramagnetic rotors. Executed in a high-density gas, it may offer an efficient way of generating macroscopic magnetic fields remotely (as shown in this work) and producing a large amount of spin-polarized electrons.

Experimental Demonstration of Coherent Control in Quantum Chaotic Systems.

We experimentally demonstrate coherent control of a quantum system, whose dynamics is chaotic in the classical limit. Interaction of diatomic molecules with a periodic sequence of ultrashort laser pulses leads to the dynamical localization of the molecular angular momentum, a characteristic feature of the chaotic quantum kicked rotor. By changing the phases of the rotational states in the initially prepared coherent wave packet, we control the rotational distribution of the final localized state and its total energy. We demonstrate the anticipated sensitivity of control to the exact parameters of the kicking field, as well as its disappearance in the classical regime of excitation.

Experimental Observation of Dynamical Localization in Laser-Kicked Molecular Rotors.

The periodically kicked rotor is a paradigm system for studying quantum effects on classically chaotic dynamics. The wave function of the quantum rotor localizes in angular momentum space, similarly to Anderson localization of the electronic wave function in disordered solids. Here, we observe dynamical localization in a system of true quantum rotors by subjecting nitrogen molecules to periodic sequences of femtosecond pulses. Exponential distribution of the molecular angular momentum-the hallmark of dynamical localization-is measured directly by means of coherent Raman scattering. We demonstrate the suppressed rotational energy growth with the number of laser kicks and study the dependence of the localization length on the kick strength. Because of its quantum coherent nature, both timing and amplitude noise are shown to destroy the localization and revive the diffusive growth of energy.

Adiabatic Field-Free Alignment of Asymmetric Top Molecules with an Optical Centrifuge.

We use an optical centrifuge to align asymmetric top SO_{2} molecules by adiabatically spinning their most polarizable O-O axis. The effective centrifugal potential in the rotating frame confines the sulfur atoms to the plane of the laser-induced rotation, leading to the planar molecular alignment that persists after the molecules are released from the centrifuge. The periodic appearance of the full three-dimensional alignment, typically observed only with linear and symmetric top molecules, is also detected. Together with strong in-plane centrifugal forces, which bend the molecules by up to 10 deg, permanent field-free alignment offers new ways of controlling molecules with laser light.

Generating long sequences of high-intensity femtosecond pulses.

We present an approach to creating pulse sequences extending beyond 150 ps in duration, comprised of 100 µJ femtosecond pulses. A quarter of the pulse train is produced by a high-resolution pulse shaper, which allows full controllability over the timing of each pulse. Two nested Michelson interferometers follow to quadruple the pulse number and the sequence duration. To boost the pulse energy, the long train is sent through a multipass Ti:sapphire amplifier, followed by an external compressor. A periodic sequence of 84 pulses of 120 fs width and an average pulse energy of 107 µJ, separated by 2 ps, is demonstrated as a proof of principle.

Magneto-Optical Properties of Paramagnetic Superrotors.

We study the dynamics of paramagnetic molecular superrotors in an external magnetic field. An optical centrifuge is used to create dense ensembles of oxygen molecules in ultrahigh rotational states. In is shown, for the first time, that the gas of rotating molecules becomes optically birefringent in the presence of a magnetic field. The discovered effect of "magneto-rotational birefringence" indicates the preferential alignment of molecular axes along the field direction. We provide an intuitive qualitative model, in which the influence of the applied magnetic field on the molecular orientation is mediated by the spin-rotation coupling. This model is supported by the direct imaging of the distribution of molecular axes, the demonstration of the magnetic reversal of the rotational Raman signal, and by numerical calculations.

Femtosecond lasing from a fluorescent protein in a one dimensional random cavity.

We present evidence of random lasing from the fluorescent protein DsRed2 embedded in a random one-dimensional cavity. Lasing is achieved when a purified protein solution, placed inside a layered random medium, is optically excited with a femtosecond pump pulse in the direction perpendicular to the plane of random layers. We demonstrate that pumping with ultrashort pulses resulted in a lasing threshold two orders of magnitude lower than that found for nanosecond excitation.

Sound emission from the gas of molecular superrotors.

We use an optical centrifuge to deposit a controllable amount of rotational energy into dense molecular ensembles. Subsequent rotation-translation energy transfer, mediated by thermal collisions, results in the localized heating of the gas and generates strong sound wave, clearly audible to the unaided ear. For the first time, the amplitude of the sound signal is analyzed as a function of the experimentally measured rotational energy and linear proportionality between the two observables is established.

Coherent anti-Stokes Raman spectroscopy in the presence of strong resonant signal from background molecules.

Spectroscopy of molecular mixtures with broadband femtosecond laser pulses often involves simultaneous excitation of multiple molecular species with close resonance frequencies. Interpreting the collective optical response typically requires Fourier analysis of time-resolved signals. We propose and demonstrate an alternative method of separating coherent Raman scattering signals from two molecular components with neighboring vibrational modes. We exploit "silence windows," which arise from coupling of the vibrational and rotational degrees of freedom in molecular dynamics. In silence windows, the detected signal stems solely from the minority species (here, CO2), while the strong resonant background from the dominant species (O2) is greatly suppressed.

Quantum resonances in selective rotational excitation of molecules with a sequence of ultrashort laser pulses.

We experimentally investigate the effect of quantum resonance in the rotational excitation of the simplest quantum rotor--a diatomic molecule. Using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study their dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect to demonstrate selective rotational excitation of two nitrogen isotopologs, (14)N(2) and (15)N(2). Moreover, by tuning the period of the pulse train in the vicinity of a fractional quantum resonance, we achieve selective rotational excitation of para- and ortho-isomers of (15)N(2).

Control of molecular rotation with a chiral train of ultrashort pulses.

Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. In this work we introduce a chiral pulse train--a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.

Population transfer between two quantum states by piecewise chirping of femtosecond pulses: theory and experiment.

We propose and experimentally demonstrate the method of population transfer by piecewise adiabatic passage between two quantum states. Coherent excitation of a two-level system with a train of ultrashort laser pulses is shown to reproduce the effect of an adiabatic passage, conventionally achieved with a single frequency-chirped pulse. By properly adjusting the amplitudes and phases of the pulses in the excitation pulse train, we achieve complete and robust population transfer to the target state. The piecewise nature of the process suggests a possibility for the selective population transfer in complex quantum systems.

Piecewise adiabatic passage with a series of femtosecond pulses.

We develop a method of executing complete population transfers between quantum states in a piecewise manner using a series of femtosecond laser pulses. The method can be applied to a large class of problems as it benefits from the high peak powers and large spectral bandwidths afforded by femtosecond pulses. The degree of population transfer is robust to a wide variation in the absolute and relative intensities, durations, and time ordering of the pulses. The method is studied in detail for atomic sodium where piecewise adiabatic population transfer, as well as the induction of Ramsey-type interferences, is demonstrated.

Pulse optimization for Raman spectroscopy with cross-correlation frequency resolved optical gating.

We propose to employ the technique of femtosecond pulse shaping for improving the performance of the recently suggested method of complete characterization of molecular vibrations, in which both the amplitude and phase of the laser induced vibrational coherence are detected with high resolution. The amplitude-phase information is retrieved from the cross-correlation frequency resolved optical gating of Raman modes. By creating rich interference pattern in the measured two-dimensional spectrogram of coherent anti-Stokes Raman scattering we enhance the accuracy of the retrieved spectral and temporal response and increase the robustness of the method against noise.

Guiding neuronal growth with light.

Control over neuronal growth is a fundamental objective in neuroscience, cell biology, developmental biology, biophysics, and biomedicine and is particularly important for the formation of neural circuits in vitro, as well as nerve regeneration in vivo [Zeck, G. & Fromherz, P. (2001) Proc. Natl. Acad. Sci. USA 98, 10457-10462]. We have shown experimentally that we can use weak optical forces to guide the direction taken by the leading edge, or growth cone, of a nerve cell. In actively extending growth cones, a laser spot is placed in front of a specific area of the nerve's leading edge, enhancing growth into the beam focus and resulting in guided neuronal turns as well as enhanced growth. The power of our laser is chosen so that the resulting gradient forces are sufficiently powerful to bias the actin polymerization-driven lamellipodia extension, but too weak to hold and move the growth cone. We are therefore using light to control a natural biological process, in sharp contrast to the established technique of optical tweezers [Ashkin, A. (1970) Phys. Rev. Lett. 24, 156-159; Ashkin, A. & Dziedzic, J. M. (1987) Science 235, 1517-1520], which uses large optical forces to manipulate entire structures. Our results therefore open an avenue to controlling neuronal growth in vitro and in vivo with a simple, noncontact technique.

Optical billiards for atoms.

One of the central paradigms for classical and quantum chaos in conservative systems is the two-dimensional billiard in which particles are confined to a closed region in the plane, undergoing elastic collisions with the walls and free motion in between. We report the first realization of billiards using ultracold atoms bouncing off beams of light. These beams create the desired spatial pattern, forming an "optical billiard." We find excellent agreement between theory and our experimental demonstration of chaotic and stable motion in optical billiards, establishing a new testing ground for classical and quantum chaos.

Recovery of classically chaotic behavior in a noise-driven quantum system.

The quantum kicked rotor is studied in a regime of high amplitude noise. A transition to diffusive behavior is observed as dynamical localization, characterized by suppressed diffusion and exponential momentum distributions, is completely destroyed by noise. With increasing noise amplitude, further transition to classical behavior is shown through an accurate quantitative analysis, which demonstrates that both the energy growth and the momentum distributions are reaching their classical limits. The importance of short-time correlations in the recovery of classically chaotic behavior is discussed.

Quantitative study of amplitude noise effects on dynamical localization

We study the motion of cold atoms in a pulsed standing wave of light, which constitutes an experimental realization of the quantum kicked rotor. This system exhibits dynamical localization, where quantum effects suppress classical momentum diffusion. As we introduce amplitude noise, the coherences that lead to localization are destroyed, resulting in restored diffusion. For high levels of noise, we find that the experiment is well described by a classical model, suggesting that classical behavior has been restored. We present a detailed experimental study of this noise-induced transition from quantum to classical behavior.