Two-photon coherent control of femtosecond photoassociation

Photoassociation with short laser pulses has been proposed as a technique to create ultracold ground state molecules. A broad-band excitation seems the natural choice to drive the series of excitation and deexcitation steps required to form a molecule in its vibronic ground state from two scattering atoms. First attempts at femtosecond photoassociation were, however, hampered by the requirement to eliminate the atomic excitation leading to trap depletion. On the other hand, molecular levels very close to the atomic transition are to be excited. The broad bandwidth of a femtosecond laser then appears to be rather an obstacle. To overcome the ostensible conflict of driving a narrow transition by a broad-band laser, we suggest a two-photon photoassociation scheme. In the weak-field regime, a spectral phase pattern can be employed to eliminate the atomic line. When the excitation is carried out by more than one photon, different pathways in the field can be interfered constructively or destructively. In the strong-field regime, a temporal phase can be applied to control dynamic Stark shifts. The atomic transition is suppressed by choosing a phase which keeps the levels out of resonance. We derive analytical solutions for atomic two-photon dark states in both the weak-field and strong-field regime. Two-photon excitation may thus pave the way toward coherent control of photoassociation. Ultimately, the success of such a scheme will depend on the details of the excited electronic states and transition dipole moments. We explore the possibility of two-photon femtosecond photoassociation for alkali and alkaline-earth metal dimers and present a detailed study for the example of calcium

Transform-limited pulses are not optimal for resonant multiphoton transitions

Maximizing nonlinear light-matter interactions is a primary motive for compressing laser pulses to achieve ultrashort transform limited pulses. Here we show how, by appropriately shaping the pulses, resonant multiphoton transitions can be enhanced significantly beyond the level achieved by maximizing the pulse's peak intensity. We demonstrate the counterintuitive nature of this effect with an experiment in a resonant two-photon absorption, in which, by selectively removing certain spectral bands, the peak intensity of the pulse is reduced by a factor of 40, yet the absorption rate is doubled. Furthermore, by suitably designing the spectral phase of the pulse, we increase the absorption rate by a factor of 7.Comment: 4 pages, 3 figure

NIR Femtosecond Control of Resonance-Mediated Generation of Coherent Broadband UV Emission

We use shaped near-infrared (NIR) pulses to control the generation of coherent broadband ultraviolet (UV) radiation in an atomic resonance-mediated (2+1) three-photon excitation. Experimental and theoretical results are presented for phase controlling the total emitted UV yield in atomic sodium (Na). Based on our confirmed understanding, we present a new simple scheme for producing shaped femtosecond pulses in the UV/VUV spectral range using the control over atomic resonance-mediated generation of third (or higher order) harmonic.Comment: 14 pages, 4 figure

Coherent control using adaptive learning algorithms

We have constructed an automated learning apparatus to control quantum systems. By directing intense shaped ultrafast laser pulses into a variety of samples and using a measurement of the system as a feedback signal, we are able to reshape the laser pulses to direct the system into a desired state. The feedback signal is the input to an adaptive learning algorithm. This algorithm programs a computer-controlled, acousto-optic modulator pulse shaper. The learning algorithm generates new shaped laser pulses based on the success of previous pulses in achieving a predetermined goal.Comment: 19 pages (including 14 figures), REVTeX 3.1, updated conten

Shot noise limited characterization of femtosecond light pulses

Probing the evolution of physical systems at the femto- or attosecond timescale with light requires accurate characterization of ultrashort optical pulses. The time profiles of such pulses are usually retrieved by methods utilizing optical nonlinearities, which require significant signal powers and operate in a limited spectral range\cite{Trebino_Review_of_Scientific_Instruments97,Walmsley_Review_09}. We present a linear self-referencing characterization technique based on time domain localization of the pulse spectral components, operated in the single-photon regime. Accurate timing of the spectral slices is achieved with standard single photon detectors, rendering the technique applicable in any spectral range from near infrared to deep UV. Using detection electronics with about $70$ ps response, we retrieve the temporal profile of a picowatt pulse train with $\sim10$ fs resolution, setting a new scale of sensitivity in ultrashort pulse characterization.Comment: Supplementary information contained in raw dat

Laser phase modulation approaches towards ensemble quantum computing

Selective control of decoherence is demonstrated for a multilevel system by generalizing the instantaneous phase of any chirped pulse as individual terms of a Taylor series expansion. In the case of a simple two-level system, all odd terms in the series lead to population inversion while the even terms lead to self-induced transparency. These results also hold for multiphoton transitions that do not have any lower-order photon resonance or any intermediate virtual state dynamics within the laser pulse-width. Such results form the basis of a robustly implementable CNOT gate.Comment: 10 pages, 4 figures, PRL (accepted

Noise auto-correlation spectroscopy with coherent Raman scattering

Ultrafast lasers have become one of the most powerful tools in coherent nonlinear optical spectroscopy. Short pulses enable direct observation of fast molecular dynamics, whereas broad spectral bandwidth offers ways of controlling nonlinear optical processes by means of quantum interferences. Special care is usually taken to preserve the coherence of laser pulses as it determines the accuracy of a spectroscopic measurement. Here we present a new approach to coherent Raman spectroscopy based on deliberately introduced noise, which increases the spectral resolution, robustness and efficiency. We probe laser induced molecular vibrations using a broadband laser pulse with intentionally randomized amplitude and phase. The vibrational resonances result in and are identified through the appearance of intensity correlations in the noisy spectrum of coherently scattered photons. Spectral resolution is neither limited by the pulse bandwidth, nor sensitive to the quality of the temporal and spectral profile of the pulses. This is particularly attractive for the applications in microscopy, biological imaging and remote sensing, where dispersion and scattering properties of the medium often undermine the applicability of ultrafast lasers. The proposed method combines the efficiency and resolution of a coherent process with the robustness of incoherent light. As we demonstrate here, it can be implemented by simply destroying the coherence of a laser pulse, and without any elaborate temporal scanning or spectral shaping commonly required by the frequency-resolved spectroscopic methods with ultrashort pulses.Comment: To appear in Nature Physic

Stable mode-locked pulses from mid-infrared semiconductor lasers

We report the unequivocal demonstration of mid-infrared mode-locked pulses from a semiconductor laser. The train of short pulses was generated by actively modulating the current and hence the optical gain in a small section of an edge-emitting quantum cascade laser (QCL). Pulses with pulse duration at full-width-at-half-maximum of about 3 ps and energy of 0.5 pJ were characterized using a second-order interferometric autocorrelation technique based on a nonlinear quantum well infrared photodetector. The mode-locking dynamics in the QCLs was modelled and simulated based on Maxwell-Bloch equations in an open two-level system. We anticipate our results to be a significant step toward a compact, electrically-pumped source generating ultrashort light pulses in the mid-infrared and terahertz spectral ranges.Comment: 26 pages, 4 figure

Prospects for precision measurements of atomic helium using direct frequency comb spectroscopy

We analyze several possibilities for precisely measuring electronic transitions in atomic helium by the direct use of phase-stabilized femtosecond frequency combs. Because the comb is self-calibrating and can be shifted into the ultraviolet spectral region via harmonic generation, it offers the prospect of greatly improved accuracy for UV and far-UV transitions. To take advantage of this accuracy an ultracold helium sample is needed. For measurements of the triplet spectrum a magneto-optical trap (MOT) can be used to cool and trap metastable 2^3S state atoms. We analyze schemes for measuring the two-photon $2^3S \to 4^3S$ interval, and for resonant two-photon excitation to high Rydberg states, $2^3S \to 3^3P \to n^3S,D$. We also analyze experiments on the singlet-state spectrum. To accomplish this we propose schemes for producing and trapping ultracold helium in the 1^1S or 2^1S state via intercombination transitions. A particularly intriguing scenario is the possibility of measuring the $1^1S \to 2^1S$ transition with extremely high accuracy by use of two-photon excitation in a magic wavelength trap that operates identically for both states. We predict a ``triple magic wavelength'' at 412 nm that could facilitate numerous experiments on trapped helium atoms, because here the polarizabilities of the 1^1S, 2^1S and 2^3S states are all similar, small, and positive.Comment: Shortened slightly and reformatted for Eur. Phys. J.

Nanoscale Processing by Adaptive Laser Pulses

We theoretically demonstrate that atomically-precise ``nanoscale processing" can be reproducibly performed by adaptive laser pulses. We present the new approach on the controlled welding of crossed carbon nanotubes, giving various metastable junctions of interest. Adaptive laser pulses could be also used in preparation of other hybrid nanostructures.Comment: 4 pages, 4 Postscript figure