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1.
Observations of intermolecular excimers in several pi-conjugated polymers and exciplexes of these polymers with tris(p-tolyl) amine are reported. It is shown that the luminescence of conjugated polymer thin films originates from excimer emission and that the generally low quantum yield is the result of self-quenching. Thus, in sufficiently dilute solution, the "single-chain" emission has a quantum yield of unity. Exciplex luminescence and exciplex-mediated charge photogeneration have much higher quantum yields than the excimer-mediated photophysical processes. These results provide a basis for understanding and controlling the photophysics of conjugated polymers in terms of supramolecular structure and morphology.  相似文献   

2.
Nanoscale semiconductor heterostructures such as tetrapods can be used to mimic light-harvesting processes. We used single-particle light-harvesting action spectroscopy to probe the impact of particle morphology on energy transfer and carrier relaxation across a heterojunction. The generic form of an action spectrum [in our experiments, photoluminescence excitation (PLE) under absorption in CdS and emission from CdSe in nanocrystal tetrapods, rods, and spheres] was controlled by the physical shape and resulting morphological variation in the quantum confinement parameters of the nanoparticle. A correlation between single-particle PLE and physical shape as determined by scanning electron microscopy was demonstrated. Such an analysis links local structural non-uniformities such as CdS bulbs forming around the CdSe core in CdSe/CdS nanorods to a lower probability of manifesting excitation energy-dependent emission spectra, which in turn is probably related to band alignment and electron delocalization at the heterojunction interface.  相似文献   

3.
Although perfect copying of unknown quantum systems is forbidden by the laws of quantum mechanics, approximate cloning is possible. A natural way of realizing quantum cloning of photons is by stimulated emission. In this context, the fundamental quantum limit to the quality of the clones is imposed by the unavoidable presence of spontaneous emission. In our experiment, a single input photon stimulates the emission of additional photons from a source on the basis of parametric down-conversion. This leads to the production of quantum clones with near-optimal fidelity. We also demonstrate universality of the copying procedure by showing that the same fidelity is achieved for arbitrary input states.  相似文献   

4.
Efficient collection and detection of fluorescence coupled with careful minimization of background from impurities and Raman scattering now enable routine optical microscopy and study of single molecules in complex condensed matter environments. This ultimate method for unraveling ensemble averages leads to the observation of new effects and to direct measurements of stochastic fluctuations. Experiments at cryogenic temperatures open new directions in molecular spectroscopy, quantum optics, and solid-state dynamics. Room-temperature investigations apply several techniques (polarization microscopy, single-molecule imaging, emission time dependence, energy transfer, lifetime studies, and the like) to a growing array of biophysical problems where new insight may be gained from direct observations of hidden static and dynamic inhomogeneity.  相似文献   

5.
We report on the electron analog of the single-photon gun. On-demand single-electron injection in a quantum conductor was obtained using a quantum dot connected to the conductor via a tunnel barrier. Electron emission was triggered by the application of a potential step that compensated for the dot-charging energy. Depending on the barrier transparency, the quantum emission time ranged from 0.1 to 10 nanoseconds. The single-electron source should prove useful for the use of quantum bits in ballistic conductors. Additionally, periodic sequences of single-electron emission and absorption generate a quantized alternating current.  相似文献   

6.
Single-photon-added coherent states are the result of the most elementary amplification process of classical light fields by a single quantum of excitation. Being intermediate between a single-photon Fock state (fully quantum-mechanical) and a coherent (classical) one, these states offer the opportunity to closely follow the smooth transition between the particle-like and the wavelike behavior of light. We report the experimental generation of single-photon-added coherent states and their complete characterization by quantum tomography. Besides visualizing the evolution of the quantum-to-classical transition, these states allow one to witness the gradual change from the spontaneous to the stimulated regimes of light emission.  相似文献   

7.
Optical emission from individual strained indium arsenide (InAs) islands buried in gallium arsenide (GaAs) was studied. At low excitation power density, the spectra from these quantum dots consist of a single line. At higher excitation power density, additional emission lines appeared at both higher and lower energies, separated from the main line by about 1 millielectron volt. At even higher excitation power density, this set of lines was replaced by a broad emission peaking below the original line. The splittings were an order of magnitude smaller than the lowest single-electron or single-hole excited state energies, indicating that the fine structure results from few-particle interactions in the dot. Calculations of few-particle effects give splittings of the observed magnitude.  相似文献   

8.
All previous experimental and theoretical studies of molecular interactions at metal surfaces show that electronically nonadiabatic influences increase with molecular velocity. We report the observation of a nonadiabatic electronic effect that follows the opposite trend: The probability of electron emission from a low-work function surface--Au(111) capped by half a monolayer of Cs--increases as the velocity of the incident NO molecule decreases during collisions with highly vibrationally excited NO(X(2)pi((1/2)), V = 18; V is the vibrational quantum number of NO), reaching 0.1 at the lowest velocity studied. We show that these results are consistent with a vibrational autodetachment mechanism, whereby electron emission is possible only beyond a certain critical distance from the surface. This outcome implies that important energy-dissipation pathways involving nonadiabatic electronic excitations and, furthermore, not captured by present theoretical methods may influence reaction rates at surfaces.  相似文献   

9.
A quantum fluid passing an obstacle behaves differently from a classical one. When the flow is slow enough, the quantum gas enters a superfluid regime, and neither whirlpools nor waves form around the obstacle. For higher flow velocities, it has been predicted that the perturbation induced by the defect gives rise to the turbulent emission of quantized vortices and to the nucleation of solitons. Using an interacting Bose gas of exciton-polaritons in a semiconductor microcavity, we report the transition from superfluidity to the hydrodynamic formation of oblique dark solitons and vortex streets in the wake of a potential barrier. The direct observation of these topological excitations provides key information on the mechanisms of superflow and shows the potential of polariton condensates for quantum turbulence studies.  相似文献   

10.
Colloidal quantum rods of cadmium selenide (CdSe) exhibit linearly polarized emission. Empirical pseudopotential calculations predict that slightly elongated CdSe nanocrystals have polarized emission along the long axis, unlike spherical dots, which emit plane-polarized light. Single-molecule luminescence spectroscopy measurements on CdSe quantum rods with an aspect ratio between 1 and 30 confirm a sharp transition from nonpolarized to purely linearly polarized emission at an aspect ratio of 2. Linearly polarized luminescent chromophores are highly desirable in a variety of applications.  相似文献   

11.
Conjugated polymers and indium arsenide-based nanocrystals were used to create near-infrared plastic light-emitting diodes. Emission was tunable from 1 to 1.3 micrometers--a range that effectively covers the short-wavelength telecommunications band--by means of the quantum confinement effects in the nanocrystals. The external efficiency value (photons out divided by electrons in) is approximately 0.5% (that is, >1% internal) and is mainly limited by device architecture. The near-infrared emission did not overlap the charge-induced absorption bands of the polymer.  相似文献   

12.
Quantum phase is not directly observable and is usually determined by interferometric methods. We present a method to map complete electron wave functions, including internal quantum phase information, from measured single-state probability densities. We harness the mathematical discovery of drum-like manifolds bearing different shapes but identical resonances, and construct quantum isospectral nanostructures with matching electronic structure but divergent physical structure. Quantum measurement (scanning tunneling microscopy) of these "quantum drums"-degenerate two-dimensional electron states on the copper(111) surface confined by individually positioned carbon monoxide molecules-reveals that isospectrality provides an extra topological degree of freedom enabling robust quantum state transplantation and phase extraction.  相似文献   

13.
Visible-stimulated emission in a semiconductor quantum dot (QD) laser structure has been demonstrated. Red-emitting, self-assembled QDs of highly strained InAlAs have been grown by molecular beam epitaxy on a GaAs substrate. Carriers injected electrically from the doped regions of a separate confinement heterostructure thermalized efficiently into the zero-dimensional QD states, and stimulated emission at approximately 707 nanometers was observed at 77 kelvin with a threshold current of 175 milliamperes for a 60-micrometer by 400-micrometer broad area laser. An external efficiency of approximately 8.5 percent at low temperature and a peak power greater than 200 milliwatts demonstrate the good size distribution and high gain in these high-quality QDs.  相似文献   

14.
A microscopic method for simulating quantum mechanical, nuclear tunneling effects in biological electron transfer reactions is presented and applied to several electron transfer steps in photosynthetic bacterial reaction centers. In this "dispersed polaron" method the fluctuations of the protein and the electron carriers are projected as effective normal modes onto an appropriate reaction coordinate and used to evaluate the quantum mechanical rate constant. The simulations, based on the crystallographic structure of the reaction center from Rhodopseudomonas viridis, focus on electron transfer from a bacteriopheophytin to a quinone and the subsequent back-reaction. The rates of both of these reactions are almost independent of temperature or even increase with decreasing temperature. The simulations reproduce this unusual temperature dependence in a qualitative way, without the use of adjustable parameters for the protein's Franck-Condon factors. The observed dependence of the back-reaction on the free energy of the reaction also is reproduced, including the special behavior in the "inverted region."  相似文献   

15.
Murr LE 《Science (New York, N.Y.)》1974,183(4121):206-208
Ordered arrays of defect aggregates in the (111) planes of natural fluorite have been observed by transmission electron microscopy. The intense blue coloration observed in corresponding sample areas after 200-kilovolt electron microscopy confirms the conclusion that these are color-center aggregates and, conversely, that color centers are primarily responsible for fluorite coloration.  相似文献   

16.
The exceptional spin coherence of nitrogen-vacancy centers in diamond motivates their function in emerging quantum technologies. Traditionally, the spin state of individual centers is measured optically and destructively. We demonstrate dispersive, single-spin coupling to light for both nondestructive spin measurement, through the Faraday effect, and coherent spin manipulation, through the optical Stark effect. These interactions can enable the coherent exchange of quantum information between single nitrogen-vacancy spins and light, facilitating coherent measurement, control, and entanglement that is scalable over large distances.  相似文献   

17.
Optical gain and stimulated emission in nanocrystal quantum dots   总被引:1,自引:0,他引:1  
The development of optical gain in chemically synthesized semiconductor nanoparticles (nanocrystal quantum dots) has been intensely studied as the first step toward nanocrystal quantum dot lasers. We examined the competing dynamical processes involved in optical amplification and lasing in nanocrystal quantum dots and found that, despite a highly efficient intrinsic nonradiative Auger recombination, large optical gain can be developed at the wavelength of the emitting transition for close-packed solids of these dots. Narrowband stimulated emission with a pronounced gain threshold at wavelengths tunable with the size of the nanocrystal was observed, as expected from quantum confinement effects. These results unambiguously demonstrate the feasibility of nanocrystal quantum dot lasers.  相似文献   

18.
We combined coherent nonlinear optical spectroscopy with nano-electron volt energy resolution and low-temperature near-field microscopy with subwavelength resolution (相似文献   

19.
We report on the generation of picosecond self-mode-locked pulses from midinfrared quantum cascade lasers, at wavelengths within the important molecular fingerprint region. These devices are based on intersubband electron transitions in semiconductor nanostructures, which are characterized by some of the largest optical nonlinearities observed in nature and by picosecond relaxation lifetimes. Our results are interpreted with a model in which one of these nonlinearities, the intensity-dependent refractive index of the lasing transition, creates a nonlinear waveguide where the optical losses decrease with increasing intensity. This favors the generation of ultrashort pulses, because of their larger instantaneous intensity relative to continuous-wave emission.  相似文献   

20.
We report on the coherent quantum state transfer from a two-level atomic system to a single photon. Entanglement between a single photon (signal) and a two-component ensemble of cold rubidium atoms is used to project the quantum memory element (the atomic ensemble) onto any desired state by measuring the signal in a suitable basis. The atomic qubit is read out by stimulating directional emission of a single photon (idler) from the (entangled) collective state of the ensemble. Faithful atomic memory preparation and readout are verified by the observed correlations between the signal and the idler photons. These results enable implementation of distributed quantum networking.  相似文献   

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