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International audience; An experimental platform operating at the level of individual quanta and providing strong light-matter coupling is a key requirement for quantum information processing. In our work, we show that hollow-core photonic bandgap fibers filled with laser-cooled atoms might serve as such a platform, despite their typical complicated birefringence properties. To this end, we present a detailed theoretical and experimental study to identify a fiber with suitable properties to achieve operation at the single-photon level. In the fiber, we demonstrate the storage and on-demand retrieval as well as the creation of stationary light pulses, based on electromagnetically induced transparency, for weak coherent light pulses down to the single-photon level with an unconditional noise floor of 0.017(4) photons per pulse. These results clearly demonstrate the prospects of such a fiber-based platform for applications in quantum information networks.

We present strong enhancements of the signal yield in third harmonic generation microscopy by seeding the optically nonlinear sample with some intensity at the third harmonic wavelength, in addition to the driving fundamental beam. By applying a third harmonic bias pulse with a power of less then 0.1% of the fundamental beam, we boost the signal yield by more than a factor of 3000, compared to the conventional third harmonic signal from the microscopy sample. The signal enhancement is most pronounced at low laser intensity and/or weak nonlinear susceptibilities. This makes the concept particularly suitable to improve the signal-to-noise ratio from samples with weak signals, e.g., as typical for applications of nonlinear microscopy. Moreover, we demonstrate improved spatial resolution in beam propagation direction by more than an order of magnitude. This exploits the dependence of our approach for enhanced third harmonic generation from inevitable dispersion in the sample. The improvement is most evident in cases, where the sample geometry allows only weak focusing.

We investigate phase-matched harmonic generation of ultrashort (picosecond) laser pulses, tuned in the vicinity of a five-photon resonance in argon, confined in a hollow-core optical waveguide. This combines resonance enhancements and tight spatial confinement to increase the conversion efficiency toward vacuum-ultraviolet radiation pulses. We demonstrate that appropriate choice of the gas pressure maintains optimal phase-matching conditions also in the presence of inevitable dynamic level shifts at high intensities. Moreover, we reveal the considerable contribution of higher-order transversal waveguide modes to the total conversion efficiency and investigate the role of cascading frequency conversion processes. Finally, we study additional signal enhancements by buffer gas admixtures. The experimental data are compared with numerical simulations, taking higher transversal waveguide modes and cascade frequency conversion into account, identifying also the potential of quasi-phase matching by polarization mode beating. Our investigations show that proper choice of experimental parameters enables significant resonance enhancements in the conversion efficiency of harmonic generation.

We report on the first observation of stationary light pulses and narrowband light storage inside a hollow-core photonic crystal fiber. Laser-cooled atoms were first loaded into the fiber core providing strong light-matter coupling. Light pulses were then stored in a collective atomic excitation using a single control laser beam. By applying a second counterpropagating control beam, a light pulse could be brought to a standstill. Our work paves the way towards the creation of strongly-correlated many-body systems with photons and applications in the field of quantum information processing.

We monitor and characterize near-surface diffusion of miscible, transparent liquids in a microfluidic device by third harmonic microscopy. The technique enables observations even of transparent or index-matched media without perturbation of the sample. In particular, we image concentrations of ethanol diffusing in water and estimate the diffusion coefficient from the third harmonic images. We obtain a diffusion coefficient D = (460 ± 30) μm2/s, which is consistent with theoretical predictions. The investigations clearly demonstrate the potential of harmonic microscopy also under the challenging conditions of transparent fluids.

article i nfo We propose a simple and powerful protocol to map an arbitrary atomic coherence between two quantum states into a population distribution of three metastable states, and later to retrieve the atomic coherence from the population distribution. The protocol applies simple sequences of radiation pulses with arbitrary temporal profile, either as coincident or as consecutive pulses. Mapping of rather short-lived atomic coherences into very long-lived atomic populations permits the prolongation of storage times (e.g. of optical information encoded in atomic coherences) by many orders of magnitude — without the need for complicated techniques to reduce homogeneous broadenings.

Spatial solitons permit optical waveguiding. This holds true for the soliton write beam (i.e. the driving laser beam), as well as for additional probe beams, which may carry optically encoded information. This feature of spatial solitons is of significant interest for applications in optical telecommunication. We pres- ent systematic experimental investigations on single and multiple spatial solitons in the infrared spectral regime (i.e. around optical telecommunication wavelengths), applied as controllable all-optical devices. In particular, we present the implementations of a Y-coupler as an optical signal divider, a switchable Y-coupler as an optical add multiplexer, and a novel design for a 1 � 3 optical beam switch, i.e. applied as a router for infrared signal beams. We report large waveguiding efficiencies up to 40% and transmis- sion rates of 90 Tbit/s in our setups. The presented experimental data are confirmed by numerical simulations.

We report on rapid adiabatic passage (RAP) in a Pr3+:Y2SiO5 crystal, cooled to cryogenic temperatures. The medium is prepared by optical pumping and spectral hole burning, creating a spectrally isolated two-level system within the inhomogeneous bandwidth of the 3H4 → 1D2 transition of the Pr3+ ions. A chirped laser pulse drives a RAP process in the medium, i.e. inverts the initial population distribution. We study the properties and dynamics of RAP by means of fluorescence detection, absorption spectroscopy and amplified spontaneous emission. Time-resolved absorption measurements serve to monitor the adiabatic population dynamics during the excitation process. In addition, we compare the results with coherent excitation at fixed laser frequency detuned from resonance, i.e. coherent population return (CPR).

We demonstrate significant enhancement of four-wave mixing in coherently driven mercury isotopes to generate vacuum-ultraviolet radiation at 125 nm. The enhancement is accomplished by preparation of the mercury atoms in a state of maximum coherence, i.e. maximum nonlinear-optical polarization, driven by Stark-chirped rapid adiabatic passage (SCRAP). In this technique, a pump laser at 313 nm excites the two-photon transition between the ground state 6s 21 S0 and the target state 7s 1 S0 in mercury. A strong, offresonant radiation field at 1064 nm generates dynamic Stark shifts. These Stark shifts serve to induce a rapid adiabatic passage process on the two-photon transition. During the process a coherent superposition of the two states is established, which enhances the nonlinear-optical polarization in the medium to the maximum possible value. The maximum coherence permits efficient four-wave mixing of a pump laser and an additional probe laser at 626 nm. The efficiency is further enhanced, as the SCRAP process allows to stimulate the complete set of different mercury isotopes to participate in the frequency conversion process. This enlarges the effective atomic density of the medium. Thus, we observe the generation of vacuum-ultraviolet radiation at 125 nm enhanced by more than one order of magnitude with respect to conventional frequency conversion. Parallel to the frequency conversion process, we monitored the evolution of the population in the medium by laser-induced fluorescence. These data demonstrate efficient coherent population transfer by SCRAP.

We report enhancement of third-harmonic generation in a nonlinear optical medium, prepared in maximum coherence by Stark-chirped rapid adiabatic passage (SCRAP). In this technique a strong off-resonant infrared radiation pulse induces an adiabatic passage process by sweeping the transition frequency of a two-photon transition in Krypton atoms through resonance with a near-resonant pump radiation pulse at 213 nm, appropriately delayed with respect to the infrared radiation. During the adiabatic passage process, a transient two-photon maximum coherence is induced, which beats with the pump laser frequency. Detrimental effects of Doppler broadening and collisional dephasing in the medium are reduced during the SCRAP process. The efficiency of third-harmonic generation, yielding vacuum-ultraviolet radiation at 71 nm is enhanced by more than one order of magnitude with respect to the case of conventional frequency conversion in an unprepared medium.

We present experimental data on quantum interferences in resonantly enhanced frequency up-conversion towards the vacuum-ultraviolet spectral regime. The process is driven in xenon atoms by ultrashort (picosecond) laser pulses. We use two simultaneous frequency conversion pathways via an excited intermediate state, i.e., fifth harmonicgenerationofthefundamentalwavelengthandfour-wavemixingofthefundamentalandtwophotonsof itssecondharmonicwavelength.Bothconversionpathwaysyieldradiationat102nm.Thetwopathwaysinterfere, depending on the relative phase of the fundamental and second harmonic. By appropriate choice of the phase we get constructive interference (resulting in increased conversion efficiency) or destructive interference (resulting in reduced conversion efficiency). The total conversion yield shows very pronounced constructive and destructive quantum interference with a visibility of roughly 90%. A stable and highly accurate phase control setup enables suchstrongquantuminterferencesformorethan260oscillationcycles.Inanextensionoftheexperiment,simultaneouslytofrequencyconversionwealsomonitorlaser-inducedfluorescenceasameasurefortheexcitationprobabilitytotheexcitedintermediatestate.Also,intheexcitationprobabilityweobservestrongquantuminterferences. As an interesting feature, a small phase lag occurs between the quantum interference patterns of frequency conversion and population transfer. This is due to an additional atomic phase acquired during frequency conversion.

The spectral width of an atomic absorption line, observed with a steady light source, typically increases as the light intensity increases, an effect known as power broadening. In this paper, we point out classes of pulsed-light observations where power broadening does not always occur. We present analytical and numerical results, supported by experimental data of coherent pulsed excitation probed by photoionization, which show that the extent of power broadening depends crucially upon the nature of excitation and the type of measurement. In particular, we show that a spectral line obtained from measurement performed after pulsed excitation exhibits no power broadening. For pulsed excitation and continuous measurement, the spectral line contains two components: a power-broadened signal collected during the excitation and an unbroadened signal collected after the excitation.

The interaction of high-intensity short pulse (fs) lasers with atomic or molecular vapors permits the conversion of visible light to intense coherent radiation in the vacuum ultraviolet spectral region. We demonstrate sum frequency mixing of a high-intensity short pulse (fs) laser with a conventional long pulse (ns) laser to extend the accessible wavelength range of harmonic generation. The mixing process does not rely on meeting resonances and can in principle be implemented with any intense short pulse (fs) laser system in any nonlinear medium. The efficiency of the sum frequency mixing process is comparable to the efficiency of harmonic generation of a similar wavelength with the high-intensity short pulse (fs) laser alone. We propose the application of conventional tunable long pulse (ns) lasers to permit the generation of broadly tunable picosecond radiation in the vacuum ultraviolet.

When one extends the conventional stimulated Raman adiabatic passage method of population transfer; involving a pump pulse preceded by a Stokes pulse, to situations in which the pump ~or pump and Stokes! interaction involves a two-photon transition, there occur unavoidable dynamic Stark shifts which prevent maintenance of the relevant resonance conditions. Such shifts can prevent the desired population transfer. We show, through numerical modeling and analytic considerations, that the detrimental effects of dynamic shifts can be compensated by a suitable choice of ~static! detunings of the carrier frequencies of the two pulses, so that population transfer can be achieved. We present simple analytic expressions for bounding the range of detunings for which population transfer can occur, and we present numerical results supporting the simple picture of the two-step linewidth. We illustrate these remarks by considering specific examples. @S1050-2947~98!09311-1#

We introduce universal broadband composite pulse sequences for robust high-fidelity population inversion in two-state quantum systems, which compensate deviations in any parameter of the driving field (e.g., pulse amplitude, pulse duration, detuning from resonance, Stark shifts, unwanted frequency chirp, etc.) and are applicable with any pulse shape. We demonstrate the efficiency and universality of these composite pulses by experimental data on rephasing of atomic coherences in a ${\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal.

We show, through analysis and numerical modeling of hydrogen and sodium, that it should be possible to transfer atomic population, with high probability, using a delayed-pulse two-photon Raman transition in which intermediate states are in the ionization continuum. We propose using auxiliary laser pulses to overcome dynamic Stark shifts that would otherwise prevent population transfer. We find that, even without such auxiliary pulses, population transfer can be improved by tuning the carrier frequencies away from the two-photon Raman resonance condition. Our computations for hydrogen predict nearly 85 percent population transfer.

The maximal storage duration is an important benchmark for memories. In quantized media, storage times are typically limited due to stochastic interactions with the environment. Also, optical memories based on electromagnetically induced transparency (EIT) suffer strongly from such decoherent effects. External magnetic control fields may reduce decoherence and increase EIT storage times considerably but also lead to complicated multilevel structures. These are hard to prepare perfectly in order to push storage times toward the theoretical limit, i.e., the population lifetime T(1). We present a self-learning evolutionary strategy to efficiently drive an EIT-based memory. By combination of the self-learning loop for optimized optical preparation and improved dynamical decoupling, we extend EIT storage times in a doped solid above 40 s. Moreover, we demonstrate storage of images by EIT for 1 min. These ultralong storage times set a new benchmark for EIT-based memories. The concepts are also applicable to other storage protocols.

We report on the preparation of a one-dimensional ultracold medium in a hollow-core photonic crystal fiber, reaching an effective optical depth of 1000(150). We achieved this extreme optical depth by transferring atoms from a magneto-optical trap into a far-detuned optical dipole trap inside the hollow-core fiber, yielding up to 2.5(3)$\times$10$^5$ atoms inside the core with a loading efficiency of $2.5(6)~\%$. The preparation of an ultracold medium of such huge optical depth paves the way towards new applications in quantum optics and nonlinear optics.

We propose and experimentally demonstrate novel types of composite sequences of half-wave and quarter-wave polarization retarders, either permitting operation at ultra-broad spectral bandwidth or narrow bandwidth. The retarders are composed of stacked standard half-wave retarders and quarter-wave retarders of equal thickness. To our knowledge, these home-built devices outperform all commercially available compound retarders, made of several birefringent materials., 5 figures, 9 pages

Driving on an analogy with the technique of composite pulses in quantum physics, we propose highly efficient broadband polarization converters composed of sequences of ordinary retarders rotated at specific angles with respect to their fast-polarization axes., 5 pages, 3 figures; check JOSA A 2011

We present experimental data on the coherent control of frequency conversion toward the vacuum-ultraviolet regime in xenon atoms, applying intense ultrashort picoseconds (ps) radiation pulses. We report on quantum interference between two resonantly enhanced frequency conversion processes (i.e., fifth harmonic generation and four-wave mixing). The conversion processes are driven by a fundamental (ps) laser pulse at 530 nm and the phase-locked second harmonic at 265 nm. Both fifth harmonic generation and four-wave mixing yield vacuum-ultraviolet radiation at 106 nm. The two frequency conversion pathways interfere with each other - either constructively or destructively, depending on the relative phase of the driving laser pulses. Thus, by variation of the relative phase, we substantially enhance or reduce the conversion efficiency (i.e., the yield of generated vacuum-ultraviolet radiation).

We report on experiments dealing with feedback-controlled pulse shaping to optimize the efficiency of light storage by electromagnetically induced transparency (EIT) in a Pr{sup 3+}:Y{sub 2}SiO{sub 5} crystal. A learning loop in combination with an evolutionary algorithm permits the automatic determination of optimal temporal profiles of intensities and frequencies in the driving laser pulses (i.e., the probe and coupling pulses). As a main advantage, the technique finds optimal solutions even in the complicated multilevel excitation scheme of a doped solid, involving large inhomogeneous broadening. The learning loop experimentally determines optimal temporal intensity profiles of the coupling pulses for a given probe pulse. The optimized intensity pulse shapes enhance the light-storage efficiency in the doped solid by a factor of 2. The learning loop also determines a fast and efficient preparation pulse sequence, which serves to optically prepare the crystal prior to light-storage experiments. The optimized preparation sequence is 5 times faster than standard preparation sequences. Moreover, the optimized preparation sequence enhances the optical depth in the medium by a factor of 5. As a consequence, the efficiency of light storage also increases by another factor of 3. Our experimental data clearly demonstrate the considerable potential of feedback-controlled pulse shaping, appliedmore » to EIT-driven light storage in solid media.« less

We have investigated the behavior of high-order stimulated Raman scattering in a highly-transient regime. We demonstrate efficient collinear generation of vibrational sidebands in molecular hydrogen and methane using two-color pumping with pulses of duration 100 fs tuned to a vibrational Raman transition. A Raman spectrum with a large bandwidth was observed, ranging from the IR to the UV. Under some conditions strong pump depletion was observed and up to five anti-Stokes sidebands were observed to have energies exceeding 10% of the transmitted pump pulse energies. A numerical simulation reproduces qualitatively and quantitatively the experimental results and allows us to explain key experimental features. The simulation also confirms that the molecular coherence in the medium is substantially increased by the two-color pumping and allows us to deduce values for the degree of material excitation. The use of this technique looks promising for efficient subfemtosecond pulse generation.

We demonstrate efficient generation of high-order anti-Stokes Raman sidebands in a highly transient regime, using a pair of approximately 100-fs laser pulses tuned to Raman resonance with vibrational transitions in methane or hydrogen. The use of this technique looks promising for efficient subfemtosecond pulse generation.

We report on the implementation of an all-solid-state optical parametric oscillator (OPO) laser system, pumped by a fiber laser, and extended by intra-cavity sum frequency generation (SFG) to provide tunable radiation with output powers well beyond 1 W in the visible regime between 605 and 616 nm. We use periodically poled sections for quasi phase-matched OPO and SFG processes, implemented on a single MgO:PPLN crystal. A Pound-Drever-Hall frequency stabilization reduces the laser linewidth to the range of 100 kHz (FWHM), determined by measurements of spectral hole burning in a rare-earth ion doped crystal as well as analysis of side-of-fringe transmission in a low finesse Fabry-Perot resonator.

We propose a method for the measurement of attosecond beating structures that result from the superposition of harmonics of laser radiation. It utilizes the phase control of the excitation probability of atoms through different interfering channels. The channels consist of multiphoton excitation by the fundamental frequency and single-photon excitation by the superposition of the harmonic fields, or alternatively, by each harmonic or frequency interval within the bandwidth of each harmonic. The method is sensitive to the relative phase of the harmonics, including phases introduced by chirp, and thus allows evaluation of the temporal structure of the superimposed harmonic fields. An experimental setup for the implementation of the method based on freestanding transmission grating is suggested as well.

We present experimental investigations, accompanied by numerical simulations on third harmonic generation microscopy at interfaces. In particular we study the variation of the emitted third harmonic intensity profile with the interface orientation. Our data confirm previous theoretical predications that only at interfaces perpendicular to the direction of the fundamental laser beam can the generated third harmonic profile exhibit a single spot in the forward direction. At interfaces parallel with the direction of the fundamental beam, the third harmonic intensity profile moves outside the forward direction and develops into a double-spot beam with a large opening angle. As an important consequence for implementations of harmonic generation microscopy, the numerical aperture of the double-spot third harmonic beam exceeds the numerical aperture of the fundamental beam.

We present systematic experimental investigations on the effects of laser polarization and interface orientation in second and third harmonic generation microscopy. We find that the laser polarization has no measurable effect on signal strength and resolution in third harmonic microscopy, while the second harmonic strongly depends upon the polarization direction of the driving laser. Moreover, we observe a strong effect of the interface orientation with respect to the laser beam direction-both in second and third harmonic generation. This affects the signal strength, as well as the obtained transversal and longitudinal resolution in microscopic imaging. As an (on the first glance) surprising feature, also surfaces parallel to the optical axis of the laser beam yield strong harmonic signal. This enables applications of harmonic microscopy in specific geometries. As an example we monitor the flow of immiscible microfluids in lateral cut by third harmonic microscopy.

We demonstrate strong enhancements of signal yield and image contrast in third-harmonic microscopy by appropriate choice of driving laser wavelength to modulate the phase-matching conditions of the conversion process by dispersion control. Tuning the laser wavelength in the range of 1010 – 1350 nm at samples containing interfaces with water and glass, we obtained large signal enhancements up to a factor of 19, and improvements in the image contrast by an order of magnitude. The effect is most pronounced at interfaces with media of small and/or not too different nonlinear optical susceptibilities, e.g., as it is the case in typical samples in harmonic microscopy. Beyond the demonstration of this new variant of third-harmonic microscopy, our findings are also of relevance to a proper choice of laser systems for harmonic microscopy setups.