Linear concentration dependence of vibrational width and vibrational dephasing paths in aqueous nitrate solutions

A theoretical model of vibrational dephasing of Raman active ions in aqueous electrolyte solutions is presented in which a probe ion is coupled to the bath by direct ion-solvent and ion-ion interactions. Expression for the vibrational width in terms of concentrations and efficiencies of the vibrational frequency modulation by ion-perturber interactions is given in the fast modulation scheme. The observed linear concentration dependence of the vibrational dephasing width of the v ₁(A'₁) mode of NO₃ ^- in aqueous solutions is reasonably well explained from this model, and efficiencies of the dephasing paths through NO₃ ^--water hydrogen bonding interaction and contact NO₃ ^--cation pair formation interaction are estimated. Anions in the solution give only a secondary effect to nitrate vibrational dephasing because of interionic repulsive forces.     

CdSe纳米晶带隙随温度变化的研究

根据带隙与吸收光谱的第一吸收峰峰位之间存在的关系,测量了粒子尺寸分别为4.0 nm和2.5 nm的CdSe纳米晶在不同温度下的吸收光谱,找出了吸收光谱第一吸收峰峰位随温度的变化关系,总结出了CdSe纳米晶的带隙随温度的变化关系.结果表明：CdSe纳米晶材料的发光器件的发光颜色取决于它的带隙.     

Size-dependence of the anharmonicities in the vibrational potential of colloidal CdSe nanocrystals

We investigated multi-phonon processes in two types of CdSe nanocrystals, spherical quantum dots and nanorods by temperature-dependent Raman spectroscopy. We find the anharmonic constants relating to the two- and three-phonon decay channels to systematically change with changing nanocrystal size. The contributions from two-phonon processes decrease with decreasing diameter, while the contributions from higher-order processes increase. The anharmonicities in the vibrational potential increase due to the phonon confinement, and we did not find a shape dependence.     

Probing solvation dynamics with femtosecond vibrational spectroscopy

We explain why solvent reorganization can induce both red- and blue-shifting of vibrational transitions of a particular probe molecule upon excitation to the S₁ electronic state. We observe with femtosecond vibrational spectroscopy, after hydrogen-bond cleavage dynamics, an additional blue shift of the carbonyl stretch of coumarin 102 of 7 cm^-1 when dissolved in chloroform. Received: 28 June 2000 / Published online: 7 August 2000     

Temperature dependence of photoluminescence from CdSe nanocrystals embedded in silica matrix

In this work, CdSe nanocrystals (NCs) embedded in SiO₂ matrix were grown by radio frequency (RF)-sputtering technique. X-ray technique was used to characterise the structural properties of the system. The NC's size was estimated to be around 4±1 nm in diameter. The temperature dependence of the photoluminescence from the CdSe/SiO₂ system showed carriers thermal exchange between the NCs and deep defects in the matrix. The evolution of the excitonic energy emission with temperature is about 10 meV in the temperature range 15-295 K. This weak shift was explained by thermal mismatch between the matrix and the NCs.     

Ultrafast dynamics of carrier-induced absorption changes in highly-excited CdSe nanocrystals

We use femtosecond time-resolved transmission spectroscopy to study the density and time dependence of transient absorption changes of CdSe nanocrystals. Our data show pronounced absorption saturation up to complete bleaching of the lowest optical transition. At high carrier density the nonlinear spectra show several peaks that can be related to the two lowest quantized electron states. Thetime dependence of the carrier-induced absorption changes indicates an ultrafast relaxation process within the strongly broadened absorption lines.     

Quantum measurement and pure dephasing

The prerequisite of quantum measurement is a transformation of an initially off-diagonal density matrix _ρmα;nβ describing an interacting measured object and measuring device into a diagonal density matrix _{ρmα;mαδmnδαβ} . The latter density matrix describes a proper mixture of states having definitem-values. On the other hand, the irreversible relaxation (towards the thermodynamic equilibrium) is also characterized by transformation of an initially off-diagonal matrix into a diagonal one. It has been shown that the process of irreversible relaxation can be used to perform quantum measurement, provided the duration Δt of the measurement is much larger thanT ₂, the phase relaxation time, and much smaller thanT ₁, the population relaxation time:T ₂ ≪ Δt ≪T ₁. Agedanken experiment describing this kind of measurement is provided. Aπ/2-pulse transforms an initials _z = −1/2 state into superposition ofs _z = ±1/2 states. The irreversible relaxation leads to the proper mixture ofs _z = 1/2 ands _z = −1/2 state. Results of the measurements are verified by the second electromagnetic pulse.     

Modification of carrier dynamics in CdSe nanocrystals by excess Cd in deposition bath

Photoexcited carrier dynamics in thin CdSe nanocrystalline films prepared by chemical bath deposition are strongly dependent on the deposition parameters. In this paper, we show how an increase in concentration of CdSO₄ in deposition bath affects the photoexcited carrier dynamics in nanocrystals. We used ultrafast absorption and photoluminescence laser spectroscopy to compare the carrier dynamics in samples prepared with and without increased CdSO₄ concentration. We have found that in the Cd-rich samples the spectral dependences of both photoluminescence and absorption dynamics are considerably less pronounced and the dynamics are slower. The observed effects were explained by the suppression of surface mediated carrier relaxation due to the passivation of individual nanocrystals by cadmium hydroxide and/or by sulphatocomplexes of Cd²⁺.     

Quantum coherent control of the vibrational dynamics of a polyatomic molecule using adaptive feedback control of a femtosecond laser

We simulate adaptive feedback control to coherently shape a femtosecond infrared laser pulse by means of a 4f-spatial light modulator in order to selectively excite the rovibrational modes of a polyatomic molecule. We preferentially populate an arbitrarily chosen upper rovibrational level by only employing these tailored temporally shaped pulses. A second laser would then allow for mode selective chemistry to interact selectively with the excited population. Alternatively the excited molecules enhanced reactivity could be exploited for selective chemistry.     

Vibration-dependent trajectories and their effects on vibrational dephasing

We show that the expression for S₁ (i.e., the first term in the expansion of the S matrix) that is essential in calculating vibration-rotation pressure-broadened shifts is not properly given in the usual Robert-Bonamy (RB) formalism. The problem resulted when they considered effects of the vibrational dephasing on S₁; they tacitly made an assumption that the trajectories of interest are vibrationally independent. As a result, the current RB expression is an approximate one. Based on a vibration-dependent trajectory model, which is physically sound, we derive the correct expression for S₁. We present numerical calculations of the broadening and shifting cross sections and of the line shape parameters for the H₂-He pair and find for this molecular system, new results differ significantly from those calculated using the existing formalism. In addition, by comparing with those derived from close coupling calculations, we find that the new results are better than the old ones. Finally, we discuss how important effects from this modification could be for other molecular systems. We conclude that for certain molecular systems where the short-range collisions are the dominant source responsible for the line widths and shifts, and in addition, the isotropic potential has small depth, the present modification is a worthwhile step to be taken in order to refine the current RB formalism. Meanwhile, for other systems it may not be necessary.     

Vibrational frequency correlation and vibrational dephasing in aqueous nitrate solutions

The vibrational frequency correlation functions

of the v ₁(A′₁) mode of NO₃ ^- ions in aqueous NH₄NO₃ solutions are calculated directly from isotropic Raman profiles, assuming that the process ω(t) is gaussian. The calculated correlation functions are oscillatory decaying functions with a time period of about 0·35 ps. A model based on the generalized Langevin theory is proposed and a theoretical correlation function, obtained by first-order truncation of Mori's continued fraction representation, is found to reproduce both the observed vibrational frequency correlation functions and the vibrational correlation functions. The observed short-time oscillation with a frequency of about 95 cm^-1 is attributed to an inter-molecular librational motion between a NO₃ ^- ion and surrounding water molecules and cations.     

Surface transformation and photoinduced recovery in CdSe nanocrystals

CdSe nanocrystals in solution and films can enter a metastable state in which the highly luminescent nanocrystals become dark. This change, which we attribute to a surface transformation, can be caused by heating or by changing the environment of the nanocrystals at room temperature. The metastable transformation is reversed upon illumination of above-band-gap light, at which point the nanocrystals are again highly luminescent.     

Resonant dephasing in the electronic Mach-Zehnder interferometer

We address the recently observed unexpected behavior of Aharonov-Bohm oscillations in the electronic Mach-Zehnder interferometer that was realized experimentally in a quantum Hall system [I. Neder, Phys. Rev. Lett. 96, 016804 (2006)10.1103/PhysRevLett.96.016804]. We argue that the measured lobe structure in the visibility of oscillations and the phase rigidity result from a strong long-range interaction between two adjacent counterpropagating edge states, which leads to a resonant scattering of plasmons. The visibility and phase shift, which we express in terms of the transmission coefficient for plasmons, can be used for the tomography of edge states.     

CdSe nanocrystals in novel phosphate glass matrix

The CdSe nanoparticles have been prepared in the novel glass matrix P₂O₅–Na₂O–ZnO–Li₂O. The prepared nanoparticles and glass matrix are characterized by differential thermal analysis, X-rays diffraction, UV–vis optical absorption, and infrared spectroscopy. X-rays diffraction and optical absorption show that both of the annealing temperature and time play an important role in nanoparticles’ growth. The well-annealed and high-temperature-annealed samples suggest Zn atoms to substitute Cd atoms to form an additional ZnSe–CdSe system. Infrared spectroscopy confirms the decrease of the Zn-content in the host glass due to growing of nanoparticles, causing long phosphate chains within.     

Nonequilibrium dephasing in an electronic Mach-Zehnder interferometer

We study nonequilibrium dephasing in an electronic Mach-Zehnder interferometer. We demonstrate that the shot noise at the beam splitter of the interferometer generates an ensemble of nonequilibrium electron density configurations and that electron interactions induce configuration-specific phase shifts of an interfering electron. The resulting dephasing exhibits two characteristic features, a lobe pattern in the visibility and phase jumps of pi, in good agreement with experimental data.     

The electronic and optical properties of a triexciton in CdSe/ZnS core/shell quantum dot nanocrystals

In the study, we aim to investigate the electronic and optical properties of single excitons, biexcions and triexcitons in a CdSe/ZnS core/shell quantum dot nanocrystal. The electronic structure has been determined by solving of the Poisson–Schrödinger equations self-consistently. In calculations, the exchange-correlation effects between identical particles have been taken into account in the frame of the local density approximation. We have demonstrated that the optical properties of triexciton systems are remarkably different from the single and biexciton systems. Absorption peaks or transition energies of the triexciton system are well separated from those of single- and bi-exciton systems. We have observed that the core-radius dependent transition energy variations of triexcitons are higher when compared with single- and bi-excitonic systems. The transition energy shifts of double and triple excitons with respect to the single exciton have been calculated as a function of the core radius and we have shown that the energy shifts are inversely proportional with the radius. We have also investigated the radius-dependent changes in binding energies and lifetimes of the structures and the comparative results have been discussed in a detail manner.