Laser pulsed emissions

The time dependence of desorption remains a little-explored but potentially useful approach for mechanistic studies. Cotter (33) has monitored secondary ion kinetic energies in a laser desorption (LD) time-of-flight instrument. Laser pulses 40 ns wide were used to desorb K+ ions from solid KC1, and the ions were sampled at variable times after the laser pulse. Emission persists for several microseconds after excitation, and secondary ion kinetic energies were found to decrease when examined at longer times after excitation. This result supports a thermal model for... 

A suitable method for a detailed investigation of stimulated emission and competing excited state absorption processes is the technique of transient absorption spectroscopy. Figure 10-2 shows a scheme of this technique. A strong femtosecond laser pulse (pump) is focused onto the sample. A second ultrashort laser pulse (probe) then interrogates the transmission changes due to the photoexcita-lions created by the pump pulse. The signal is recorded as a function of time delay between the two pulses. Therefore the dynamics of excited state absorption as... 

Figure 10-8. Emission spectra of a free standing film of a blend system consisting of 0.9% MEH-PPV in polystyrene with ca. I011 cm 3 TiOj-particlcs. The nanoparlicles act as optical scattering centers. The emission spectrum is depicted for two different excitation pulse energies. Optical excitation was accomplished with laser pulses of duration I Ons and wavelength 532 nm (according to Ref. 171).

Figure 10-12. Lcfi hand side Slruclure of a PPV microcavily. A thin film of ihe conjugated polymer is deposited on top of a highly reflective distributed Bragg refieclor (DBR). The second mirror is then fabricated by evaporation of a silver layer. Right hand side Emission spectra of the microcavily at excitation cnetgics or 0.0S pJ (dashed line) and l. l pJ (solid line), respectively. Laser pulses ol duration 200-300 ps and a wavelength of 355 nm were used for optical excitation (according to Ref. [39]).

Figure 9-29. (a) Emission of" ni-Ll PP al dilTcrenl exclusion laser pulse energies, (b) Full width ai half maximum and peak position ill" ihe m-LPPP emission versus cxcilalion laser pulse energy. 

Figure 10-5. Transient transmission changes AV/Po in PPV for different lime delays between the pump and probe pulse. The pump pulse is a 100 fs laser pulse at 325 nm obtained by frequency doubling ol amplified dye laser pulses, (a) and (b) correspond to different sides of a PPV-film. The spectra in (a) were obtained lor the unoxidized side of the sample while the set of spectra in (b) was measured for the oxidized side of the same sample. The main differences observed are a much lower stimulated emission effect for the oxidized side. The two bottom spectra depict the PL-spectra for comparison. The dashed line indicates the optical absorption (according to Kef. (281).

The ability to create and observe coherent dynamics in heterostructures offers the intriguing possibility to control the dynamics of the charge carriers. Recent experiments have shown that control in such systems is indeed possible. For example, phase-locked laser pulses can be used to coherently amplify or suppress THz radiation in a coupled quantum well [5]. The direction of a photocurrent can be controlled by exciting a structure with a laser field and its second harmonic, and then varying the phase difference between the two fields [8,9]. Phase-locked pulses tuned to excitonic resonances allow population control and coherent destruction of heavy hole wave packets [10]. Complex filters can be designed to enhance specific characteristics of the THz emission [11,12]. These experiments are impressive demonstrations of the ability to control the microscopic and macroscopic dynamics of solid-state systems. 

The purpose of this work is to demonstrate that the techniques of quantum control, which were developed originally to study atoms and molecules, can be applied to the solid state. Previous work considered a simple example, the asymmetric double quantum well (ADQW). Results for this system showed that both the wave paeket dynamics and the THz emission can be controlled with simple, experimentally feasible laser pulses. This work extends the previous results to superlattices and chirped superlattices. These systems are considerably more complicated, because their dynamic phase space is much larger. They also have potential applications as solid-state devices, such as ultrafast switches or detectors. 

Photoinduced oxidation of 1,4-dimethoxybenzene (DMB) and tetrahydrofuran (THF) by [Au(C N N-dpp)Cl]+ in acetonitrile upon UV/Vis irradiation have been observed. The time-resolved absorption spectrum recorded 12 (xs after excitation of [Au(C N N-dpp)Cl] with a laser pulse at 35 5 nm showed the absorption band of the DMB radical cation at 460nm, whereas upon excitation at 406 nm in the presence of THF, a broad emission characteristic of the protonated salt of 2,9-diphenyl-l,10-phenanthroline (Hdpp ) developed at 500 nm. 

In addition to the surface/interface selectivity, IR-Visible SFG spectroscopy provides a number of attractive features since it is a coherent process (i) Detection efficiency is very high because the angle of emission of SFG light is strictly determined by the momentum conservation of the two incident beams, together with the fact that SFG can be detected by a photomultiplier (PMT) or CCD, which are the most efficient light detectors, because the SFG beam is in the visible region, (ii) The polarization feature that NLO intrinsically provides enables us to obtain information about a conformational and lateral order of adsorbed molecules on a flat surface, which cannot be obtained by traditional vibrational spectroscopy [29-32]. (iii) A pump and SFG probe measurement can be used for an ultra-fast dynamics study with a time-resolution determined by the incident laser pulses [33-37]. (iv) As a photon-in/photon-out method, SFG is applicable to essentially any system as long as one side of the interface is optically transparent. 

We consider a model for the pump-probe stimulated emission measurement in which a pumping laser pulse excites molecules in a ground vibronic manifold g to an excited vibronic manifold 11 and a probing pulse applied to the system after the excitation. The probing laser induces stimulated emission in which transitions from the manifold 11 to the ground-state manifold m take place. We assume that there is no overlap between the two optical processes and that they are separated by a time interval x. On the basis of the perturbative density operator method, we can derive an expression for the time-resolved profiles, which are associated with the imaginary part of the transient linear susceptibility, that is,... 

The most direct and easy way consists in focusing the laser pulse onto a solid target and to collect the radiation emitted by the produced plasma. The wide emitted spectrum extends from infrared to X-rays and it is produced by different physical mechanisms Bremsstrahlung, recombination, resonant lines, K-shell emission from neutral (or partially ionized) atoms. In particular, this latter mechanism has been recognized, since a decade, as a way of producing ultrashort monochromatic radiation pulses at energy up to several keV. 

---