Single Ultrafast Pulse Research Articles

Dissociation of chlorobromomethane molecules coherently regulated by ultrafast strong field

Coherent control of molecular dissociation in ultrafast strong fields has received considerable attention in various scientific disciplines, such as atomic and molecular physics, physical chemistry, and quantum control. Many fundamental issues still exist regarding the understanding of phenomena, exploration of mechanisms, and development of control strategies. Recent progress has shown that manipulating the spectral phase distribution of a single ultrafast strong ultraviolet laser pulse while maintaining the the same spectral amplitude distribution can effectively control the total dissociation probability and branching ratios of molecules initially in the ground state. In this work, the spectral phase control of the photodissociation reaction of chlorobromomethane (CH<sub>2</sub>BrCl) is studied in depth by using a time-dependent quantum wave packet method, focusing on the influence of the initial vibrational state on the dissociation reaction. The results show that modifying the spectral phase of a single ultrafast pulse does not influence the total dissociation probability or branching ratio in the weak field limit. However, these factors exhibit significant dependence on the phase of the single ultrafast pulse spectrum under the strong field limit. By analyzing the population distribution of vibrational states in the ground electronic state, we observe that chirped pulses can effectively regulate the resonance Raman scattering (RRS) phenomenon induced in strong fields, thereby selectively affecting the dissociation probability and branching ratio based on initial vibrational states. Furthermore, we demonstrate that by selecting an appropriate initial vibration state and controlling both the value and sign of the chirp rate, it is possible to achieve preferential cleavage of Cl+CH<sub>2</sub>Br bonds. This study provides new insights into understanding of ultrafast coherent control of photodissociation reactions in polyatomic molecules.

Experimental demonstration of single-shot chirped pulse digital holography

We experimentally demonstrated single-shot chirped pulse digital holography which can be used for measuring the sequence of ultrafast optical wavefronts in a relatively simple setup. In this method, multiple ultrafast object pulses and a chirped reference pulse are obtained from a single ultrafast pulse and these pulses are interfered to record a digital hologram and optical wavefronts at different times can be reconstructed separately from the recorded hologram. In experiment, two optical wavefronts obtained by a 35 fs pulse with the time separation of 3.7 ps were recorded and reconstructed successfully.

Single Broadband Phase-Shaped Pulse Stimulated Raman Spectroscopy for Standoff Trace Explosive Detection.

Recent success with trace explosives detection based on the single ultrafast pulse excitation for remote stimulated Raman scattering (SUPER-SRS) prompts us to provide new results and a Perspective that describes the theoretical foundation of the strategy used for achieving the desired sensitivity and selectivity. SUPER-SRS provides fast and selective imaging while being blind to optical properties of the substrate such as color, texture, or laser speckle. We describe the strategy of combining coherent vibrational excitation with a reference pulse in order to detect stimulated Raman gain or loss. A theoretical model is used to reproduce experimental spectra and to determine the ideal pulse parameters for best sensitivity, selectivity, and resolution when detecting one or more compounds simultaneously.

Serial snapshot crystallography with a non-monochromatic microbeam

X-ray free-electron laser (XFEL) sources create X-ray pulses of unprecedented brilliance and open up new possibilities for the structural characterization of crystalline materials. By exposing a small crystallite (100nm-10μm) to a single ultrafast pulse, a diffraction pattern can be obtained before the crystal is damaged. If such single-pulse diffraction patterns, collected sequentially on many randomly oriented crystallites, are combined, it is possible to determine the structure of the material accurately [1]. One of the drawbacks of this approach is that only a single position of the Ewald sphere is accessed in each pattern, so, because reflections have a finite width, the diffraction condition is not satisfied completely for any of the reflections recorded. The new XFEL source that is being developed in Switzerland (SwissFEL) will provide a broad-bandpass mode with an energy bandwidth of about 4% [2]. By using the full energy range of the SwissFEL beam, a new option for structural studies of crystalline materials becomes possible. In a recent study based on simulated data, we showed that a diffraction experiment with stationary crystallites in such an `extra pink' beam not only increases the number of reflection intensities that can be collected in a single shot, but also overcome the problem of `partial reflection' measurement [3]. To test the viability of the data processing with experimental data, attempts to simulate this 4% bandpass have been carried out on SNBL at ESRF and on the microXAS beamline at SLS. On SNBL, a single crystal was rotated over 360° and a continuous scan of the monochromator over the 4% energy range was performed every 1°. At SLS, a mirror was used to cut off the higher energies of the undulator beam and the energy threshold of a Pilatus detector to eliminate the lower ones. With this setup, a series of randomly oriented crystallites were measured. A comparison of the analysis of these datasets will be presented.

Fluctuation properties of acoustic phonons generated by ultrafast optical excitation of a quantum dot

We study theoretically the fluctuation properties of acoustic phonons created in a semiconductor quantum dot after ultrafast optical excitation. An excitation with a single ultrafast pulse creates an exciton confined to the quantum dot, which is coupled to longitudinal acoustic phonons. This leads to the formation of a polaron in the quantum dot accompanied by the emission of a phonon wave packet. We show that the fluctuations of the lattice displacement associated with the wave packet after a single laser pulse excitation in resonance with the exciton transition are always larger than their respective vacuum values. Manipulating the exciton with a second pulse can result in a reduction of the fluctuations below their vacuum limit, which means that the phonons are squeezed. We show that the squeezing properties of the wave packet strongly depend on the relative phase and the time delay between the two laser pulses.

Ultrafast Gates for Single Atomic Qubits

We demonstrate single-qubit operations on a trapped atom hyperfine qubit using a single ultrafast pulse from a mode-locked laser. We shape the pulse from the laser and perform a π rotation of the qubit in less than 50 ps with a population transfer exceeding 99% and negligible effects from spontaneous emission or ac Stark shifts. The gate time is significantly shorter than the period of atomic motion in the trap (Ω(Rabi)/ν(trap)>10(4)), demonstrating that this interaction takes place deep within the strong excitation regime.

Demonstrating coherent control inR85b2using ultrafast laser pulses: A theoretical outline of two experiments

Calculations relating to two experiments that demonstrate coherent control of preformed rubidium-85 molecules in a magneto-optical trap using ultrafast laser pulses are presented. In the first experiment, it is shown that pre-associated molecules in an incoherent mixture of states can be made to oscillate coherently using a single ultrafast pulse. A mechanism that can transfer molecular population to more deeply bound vibrational levels is used in the second. Optimal parameters of the control pulse are presented for the application of the mechanism to molecules in a magneto-optical trap. The calculations make use of an experimental determination of the initial state of molecules photoassociated by the trapping lasers in the magneto-optical trap and use shaped pulses consistent with a standard ultrafast laser system.

Ultrafast soft X-ray scattering and reference-enhanced diffractive imaging of weakly scattering nanoparticles

We report the first successful reconstruction of the real space image from coherent X-ray diffraction patterns of membrane-supported nanoparticles using single ultrafast pulses. The particles consisted of 145-nm spherical polystyrene spheres that were size-selected by differential mobility analysis. We investigated the dependence of signal intensity on the number of spherical nanoparticles irradiated by single ultrafast pulses at the FLASH FEL facility. We demonstrate detection of as few as two 145-nm diameter particles irradiated by a single 32 nm fs-long FLASH pulse focused to 2.4 J cm −2. In this case the noise in the diffraction pattern, due to photon-counting statistics and scattering from the supporting silicon nitride membrane, was the largest contributor to the recorded intensity. We were able to reconstruct high-resolution images of the nanoparticles using a strong scattering reference object to aid the phase retrieval of the coherent diffraction pattern. This method of reference-enhanced diffractive imaging may allow the imaging of weakly scattering objects at FLASH and other future X-ray FEL sources.

Generation of microwave pulses by optoelectronically switched resonators

The generation of ultrashort pulses or microwave bursts by optoelectronically switched transmission line resonators is investigated numerically and experimentally. When using a dc charging source, single ultrafast pulses can be generated, shorter than the laser pulse width and the carrier relaxation time of the photoconductor used. Electrical pulses shorter than 41 ps are obtained from a 430 ps dye laser pulse. When using a microwave CW signal as input, bursts with higher output power than the input power are generated. Preliminary experiments demonstrate this kind of power enhancement.