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

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

Photonics - An atomic dimmer switch

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/62775/1/396217a0.pd

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

Problems and Aspects of Energy-Driven Wavefunction Collapse Models

Four problematic circumstances are considered, involving models which describe dynamical wavefunction collapse toward energy eigenstates, for which it is shown that wavefunction collapse of macroscopic objects does not work properly. In one case, a common particle position measuring situation, the apparatus evolves to a superposition of macroscopically distinguishable states (does not collapse to one of them as it should) because each such particle/apparatus/environment state has precisely the same energy spectrum. Second, assuming an experiment takes place involving collapse to one of two possible outcomes which is permanently recorded, it is shown in general that this can only happen in the unlikely case that the two apparatus states corresponding to the two outcomes have disjoint energy spectra. Next, the progressive narrowing of the energy spectrum due to the collapse mechanism is considered. This has the effect of broadening the time evolution of objects as the universe evolves. Two examples, one involving a precessing spin, the other involving creation of an excited state followed by its decay, are presented in the form of paradoxes. In both examples, the microscopic behavior predicted by standard quantum theory is significantly altered under energy-driven collapse, but this alteration is not observed by an apparatus when it is included in the quantum description. The resolution involves recognition that the statevector describing the apparatus does not collapse, but evolves to a superposition of macroscopically different states.Comment: 17 page

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

Coherent Control of Multiphoton Transitions with Femtosecond pulse shaping

We explore the effects of ultrafast shaped pulses for two-level systems that do not have a single photon resonance by developing a multiphoton density-matrix approach. We take advantage of the fact that the dynamics of the intermediate virtual states are absent within our laser pulse timescales. Under these conditions, the multiphoton results are similar to the single photon and that it is possible to extend the single photon coherent control ideas to develop multiphoton coherent control.Comment: 13 pages, 7 figures. submitted to PR

Ultrashort-pulse laser with an intracavity phase shaping element

A novel ultrashort-pulse laser cavity configuration that incorporates an intracavity deformable mirror as a phase control element is reported. A user-defined spectral phase relation of 0.7 radians relative shift could be produced at around 1035 nm. Phase shaping as well as pulse duration optimization was achieved via a computer-controlled feedback loop

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

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