Tunneling induced quantum interference experienced by an incident probe in asymmetric double quantum wells can easily be modulated by means of an external control light beam. This phenomenon, which is here examined within the dressed-state picture, can be exploited to devise a novel all-optical ultrafast switch. For a suitably designed semiconductor heterostructure, the switch is found to exhibit frequency bandwidths of the order of 0.1 THz and response and recovery times of about 1 ps. DOI: 10.1103/PhysRevLett.95.057401 PACS numbers: 78.67.De, 42.50.Gy, 42.50.Hz, 78.66.Fd Transmission and switching of data using all-optical devices is currently the ultimate goal of most telecommunication research. To build all-optical networking systems, optical analogues of existing microelectronics devices must clearly be found. Interesting proposals toward the realization of fast switches, for instance, have already been brought forward whereas important steps toward their actual implementation are now being made. Schemes based on dipole-dipole interactions [1], nonlinear Bragg diffraction [2], photonic band-gap materials [3], as well as those most recent ones based on quantum interference in atomic media [4 -7] all seem to be quite promising.This Letter describes a proof-of-principle study demonstrating that tunable tunneling induced quantum interference in asymmetric quantum wells can be exploited to devise an efficient new mechanism for ultrafast and broadband all-optical switching working at low temperatures (T 10 K). Unlike most familiar switching schemes based on photo-induced changes of the medium macroscopic refractive index [3] or other less usual ones based instead on virtual excitation of spin-polarized excitons [8] or on switchable mirrors made of thin polycrystalline films [9], this mechanism relies on quantum interference and hence it is quite sensitive. Quantum interference based phenomena such as, e.g., coherent population trapping [10], electromagnetically induced transparency [11], lasing without inversion [12], and light speed reduction [13] have recently attracted considerable attention. For many potential applications, solid-state solutions to implement these effects, first predicted and observed in dilute atomic media, are preferred and are now being sought after. In solid media [14] only few proposals followed the original idea of making use of quantum interference to devise an optical switch, first suggested [4] to work and recently observed [6] on a four-level atomic system.We investigate the steady-state and transient behavior of a weak probe light signal incident upon an asymmetric quantum well. The probe can be stopped in the presence of an external control switch beam but made instead to propagate with little absorption when the switch beam is off. The different response depends, respectively, on whether tunneling induced quantum interference is quenched or well developed. Such a control of quantum interference hinges on the creation of a new dipole allowed intersubband transition. Large pro...

The full UV-visible dielectric tensor and the corresponding directions of the principal axes of triclinic tetracene crystals are reported as deduced either by polarized absorption and ellipsometry measurements or by calculations based on the molecular and crystallographic data. The results allow the attribution of the polarized bands observed in both absorption and photoluminescence emission spectra. In particular, the spectral line shape and polarization of the emission are found to depend on the sample thickness, and the effect is attributed to the modification of the state of polarization of the emitted light during its propagation inside the crystal. Indeed, the directions of polarization of the lowest optical transitions and the directions of the principal axes of the dielectric tensor are demonstrated not to coincide, in contrast to the assumptions typically made in the literature, thus causing the mixed transverse/longitudinal character of light propagation.

Exciton-phonon (EP) coupling in molecular aggregates is reexamined in cases where extended intermolecular interactions result in low-energy excitons with high effective masses. The analysis is based on a single intramolecular vibrational mode with frequency omega0 and Huang-Rhys factor lambda2. When the curvature Jc at the exciton band bottom is much smaller than the free-exciton Davydov splitting W, the strength of the EP coupling is determined by comparing the nuclear relaxation energy lambda2omega0 with the curvature. In this way, weak (lambda2omega0<<4piJc), intermediate I (lambda2omega0 approximately 4piJc), and strong I (lambda2omega0>>4piJc) coupling regimes are introduced. The conventional intermediate (lambda2omega0 approximately W) and strong (lambda2omega0>>W) EP coupling regimes originally defined by Simpson and Peterson [J. Chem. Phys. 26, 588 (1957)] are based solely on the Davydov splitting and are referred to here as intermediate II and strong II regimes, respectively. Within the intermediate I and strong I regimes the near degeneracy of the low-energy excitons allows efficient nonadiabatic coupling, resulting in a spectral splitting between the b- and ac-polarized first replicas in the vibronic progression characterizing optical absorption. Such spectral signatures are clearly observed in OT4 thin films and crystals, where splittings for the lowest energy mode with omega0=161 cm(-1) are as large as 30 cm(-1) with a small variation due to sample disorder. Numerical calculations using a multiphonon BO basis set and a Hamiltonian including linear EP coupling yield excellent agreement with experiment.

International audienceThe optical response of rubrene crystals is described by providing the full UV-VIS dielectric tensor. Consistently with the molecular and crystal symmetries, the lowest crystal transition originates from an Au molecular transition, it is polarized along the c axis (normal to the larger crystal face), and it is the origin of the emission, which is self-guided towards the edge where the corresponding polarization and intensity angular distribution are detected. By contrast, the Bu molecular transitions give rise to Davydov states described by the other two components of the diagonal dielectric tens

Polarized superradiant emission and exciton delocalization in tetracene single crystals are reported. Polarization-, time-, and temperature-resolved spectroscopy evidence the complete polarization of the zero-phonon line of the intrinsic tetracene emission from both the lower (F state) and the upper (thermally activated) Davydov excitons. The superradiance of the F emission is substantiated by a nearly linear decrease of the radiative lifetime with temperature, being fifteen times shorter at 30 K compared to the isolated molecule, with an exciton delocalization of about 40 molecules.

Exciton-phonon (EP) coupling in molecular crystals is investigated in the case where two intramolecular vibrational modes are involved and a theoretical model is presented which applies when one of the modes is strongly coupled to crystal excitons. The model is used to simulate the low energy portion of the absorption spectra of quaterthiophene (4T) single crystals, for which we find it appropriate to consider a low energy vibrational mode at 161 cm(-1) and an effective strongly coupled high energy mode at 1470 cm(-1). Our numerical results demonstrate that the high energy mode renormalizes the excitonic band, thereby strongly affecting the environment seen by the low energy mode and the overall EP coupling regime. Numerical simulations also confirm the existence of the new coupling regimes "intermediate-I" and "strong-I" already introduced for oligothiophene aggregates [Spano et al., J. Chem. Phys. 127, 184703 (2007)], which arise as a consequence of the large effective mass of low energy excitons in 4T crystals. Comparison with experimental high resolution absorption spectra is also reported and shown to support the model predictions.

We report a combined spectroscopic and structural study of polymorphism of 1,1,4,4-tetraphenyl-1,3-butadiene (TPB) blue luminescent crystals. We have identified two polymorphs, which can be grown by crystallization of the vapor. The first, α-TPB, has the monoclinic noncentrosymmetric structure (P21, two molecules per unit cell), whose lattice parameters have already been reported in the literature. The second, β-TPB, is a new polymorph, monoclinic centrosymmetric (P21/c, four molecules per unit cell). The previously reported triclinic structure, γ-TPB, has not been identified in samples grown by the physical vapor transport method. The effects of the different molecular configuration and packing of α- and β-TPB on Raman scattering, IR, and UV−vis optical properties are discussed.

The impact of exciton-vibrational coupling involving fast and slow vibrational modes on absorption and emission in molecular H-aggregates is investigated using a multimode Holstein Hamiltonian. For H-aggregates composed of rigid molecules the radiative decay rate is rigorously zero due to the asymmetry of the lowest energy exciton. Increasing the Huang-Rhys factors of the coupled modes results in an increase of the radiative efficiency through increased sideband emission. Coupling to a spectrally unresolved slow mode leads to an apparent increase in the 0-0 intensity of the vibronic progression of the fast mode, thereby mimicking a distribution of molecular transition frequencies (diagonal disorder). In the intermediate coupling regime, the radiative efficiency of the aggregate exceeds the sum of the fast-mode-only and slow-mode-only radiative efficiencies. The mechanism underlying the synergistic enhancement of the radiative yield is similar to that which causes spectral splitting in the absorption spectrum of quaterthiophene crystals. [L. Silvestri et al., J. Chem. Phys. 130, 234701 (2009)]. The results here qualitatively account for the robust emission efficiency of hexaphenyl microcrystallites where the slow torsional motion involving the interphenyl dihedral angle in conjunction with the fast ring breathing mode conspire to enhance the quantum yield.