Oscillation coherent

Calculations within tire framework of a reaction coordinate degrees of freedom coupled to a batli of oscillators (solvent) suggest tliat coherent oscillations in the electronic-state populations of an electron-transfer reaction in a polar solvent can be induced by subjecting tire system to a sequence of monocliromatic laser pulses on tire picosecond time scale. The ability to tailor electron transfer by such light fields is an ongoing area of interest [511 (figure C3.2.14). 

Evans D G, Coalson R D, Kim H J and Dakhnovskii Y 1995 Inducing coherent oscillations in an electron transfer dynamics of a strongly dissipative system with pulsed monochromatic light Phys. Rev. Lett. 75 3649... 

Aside from merely calculational difficulties, the existence of a low-temperature rate-constant limit poses a conceptual problem. In fact, one may question the actual meaning of the rate constant at r = 0, when the TST conditions listed above are not fulfilled. If the potential has a double-well shape, then quantum mechanics predicts coherent oscillations of probability between the wells, rather than the exponential decay towards equilibrium. These oscillations are associated with tunneling splitting measured spectroscopically, not with a chemical conversion. Therefore, a simple one-dimensional system has no rate constant at T = 0, unless it is a metastable potential without a bound final state. In practice, however, there are exchange chemical reactions, characterized by symmetric, or nearly symmetric double-well potentials, in which the rate constant is measured. To account for this, one has to admit the existence of some external mechanism whose role is to destroy the phase coherence. It is here that the need to introduce a heat bath arises. 

Coupling to these low-frequency modes (at n < 1) results in localization of the particle in one of the wells (symmetry breaking) at T = 0. This case, requiring special care, is of little importance for chemical systems. In the superohmic case at T = 0 the system reveals weakly damped coherent oscillations characterised by the damping coefficient tls (2-42) but with Aq replaced by A ft-If 1 < n < 2, then there is a cross-over from oscillations to exponential decay, in accordance with our weak-coupling predictions. In the subohmic case the system is completely localized in one of the wells at T = 0 and it exhibits exponential relaxation with the rate In k oc - hcoJksTY ". 

Steriade, M (1999) Coherent oscillations and short-term plasticity in corticothalamic networks. 

A. and Wrachtrup, A. (2004) Observation of coherent oscillations in a single electron spin. J. Phys. Rev. Lett, 92,... 

Figure 7.2 Schematic representation of coherent oscillations between states 0) and 1) of a qubit. For an electron spin placed in a dc magnetic field, oscillations can be induced via the application of an external radio frequency (rf) pulse resonant with the Zeeman energy. The amplitude 8 of the...

Averin DV, Likharev KK (1986) Coulomb blockade of tunneling, and coherent oscillations in small tunnel junctions. J Low Temp Phys 62 345-372... 

The coherent oscillation of the A g mode was a cosine function of time (Fig. 2.8) [21,24-26]. Recent X-ray measurements demonstrated a clear shift in the equilibrium position at photoexcitation [35], as we will see in the next chapter. These results confirmed the displacive generation of coherent A g phonons, as discussed in Sect. 2.2.2. In contrast, the coherent oscillation of the Eg mode was a sine function of time, and its amplitude exhibited a cos 2ip dependence on the pump polarization angle ip. Both features indicated the ISRS generation of the coherent Eg phonons [21,25],... 

Silicon is a model for the fundamental electronic and mechanical properties of Group IV crystals and the basic material for electronic device technology. Coherent optical phonons in Si revealed the ultrafast formation of renormalized quasiparticles in time-frequency space [47]. The anisotropic transient reflectivity of n-doped Si(001) featured the coherent optical phonon oscillation with a frequency of 15.3 THz, when the [110] crystalline axis was parallel to the pump polarization (Fig. 2.11). Rotation of the sample by 45° led to disappearance of the coherent oscillation, which confirmed the ISRS generation,... 

The earliest control experiments were performed in double- (or multiple-) pump and probe scheme on optical phonons generated via ISRS in transparent materials by Nelson and coworkers [24,25], Shortly later, similar experiments were carried out on coherent phonons generated in semiconductors via TDFS by Dekorsy and coworkers [26], and on those generated in semimetals via DECP by Hase and coworkers [27] (Fig. 2.1 in the previous chapter). These experiments demonstrated that the amplitude of the coherent oscillation can be controlled by varying the temporal separation At between the two pump pulses. At = nT leads to the maximum enhancement of the amplitude with an integer n and the phonon period T, while At = (n + 1/2)T results in complete cancelation. 

Fig. 3.11. Left spectrum of the tailored pump beam for different spectral separations Aw CC2 — oji between two spectral packets (oJi and Lof). The bottom case is resonant to the E2 phonon frequency l o- Right transient transmittance of GaN excited with the tailored pump pulses, showing the enhancement of coherent oscillation of the E2 phonon for u) — u)2 — Oo- From [28]...

Double pump experiments on an organic charge transfer complex TTF-CA by Iwai and coworkers demonstrated a new class of coherent control on a strongly correlated electron-lattice system [44]. While the amplitude of the coherent oscillation increased linearly with pump fluence for single pump experiments, the amplitude in the double pump experiments with a fixed pulse interval At = T exhibited a strongly super-linear fluence dependence (Fig. 3.16). The striking difference between the single- and double-pulse results indicated a cooperative nature of the photo-induced neutral-ionic transition. 

Figure 15.31 Coherent oscillation in l-V characteristics observed on a Pt nanoparticle/mesoporous silica film at 4.2 K.

The bath response function is usually associated with a characteristic correlation or memory time, t, which separates the non-Markovian (t t ) and the Markovian (t t ) temporal regimes, for example, 0(t) a Within the bath memory time, the bath modes oscillate coherently and in unison, and maintain memory of their interaction with the system, whereas after the correlation time has passed, the modes lose their coherent oscillations and forget their prior interactions [94]. 

Abstract Ultrafast photoreactions in PNS of PYP have been studied by means of fs fluorescence up conversion method. Conclusions obtained are (a) Photoreaction in PNS (chromophore twisting) occurs from vibrationally unrelaxed fluorescence state and coherent oscillations in the fluorescence decay curves have been observed for the first time, (b) Comparative studies on fluorescence dynamics of mutants and w.-t. PYP have proved that the w.-t. PYP is best engineered for the ultrafast reaction, (c) The coherent oscillations in the fluorescence decay completely disappeared and the reaction was much slower in the denatured state, demonstrating the supremely important role of PNS for the photoreaction. 

Figure 6. Restricted and dissipative IVR observed for an anthracene beam at a rotational temperature of -3 K. Note the in-phase and out-of-phase nature of the coherent oscillations (top).

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