Concept: Photoelectric effect
Gedankenexperiments have consistently played a major role in the development of quantum theory. A paradigmatic example is Wheeler’s delayed-choice experiment, a wave-particle duality test that cannot be fully understood using only classical concepts. We implement Wheeler’s idea along a satellite-ground interferometer that extends for thousands of kilometers in space. We exploit temporal and polarization degrees of freedom of photons reflected by a fast-moving satellite equipped with retroreflecting mirrors. We observe the complementary wave- or particle-like behaviors at the ground station by choosing the measurement apparatus while the photons are propagating from the satellite to the ground. Our results confirm quantum mechanical predictions, demonstrating the need of the dual wave-particle interpretation at this unprecedented scale. Our work paves the way for novel applications of quantum mechanics in space links involving multiple photon degrees of freedom.
Surface plasmon polaritons can confine electromagnetic fields in subwavelength spaces and are of interest for photonics, optical data storage devices and biosensing applications. In analogy to photons, they exhibit wave-particle duality, whose different aspects have recently been observed in separate tailored experiments. Here we demonstrate the ability of ultrafast transmission electron microscopy to simultaneously image both the spatial interference and the quantization of such confined plasmonic fields. Our experiments are accomplished by spatiotemporally overlapping electron and light pulses on a single nanowire suspended on a graphene film. The resulting energy exchange between single electrons and the quanta of the photoinduced near-field is imaged synchronously with its spatial interference pattern. This methodology enables the control and visualization of plasmonic fields at the nanoscale, providing a promising tool for understanding the fundamental properties of confined electromagnetic fields and the development of advanced photonic circuits.
Multiple exciton generation (MEG) is a process that can occur in semiconductor nanocrystals, or quantum dots (QDs), whereby absorption of a photon bearing at least twice the bandgap energy produces two or more electron-hole pairs. Here, we report on photocurrent enhancement arising from MEG in lead selenide (PbSe) QD-based solar cells, as manifested by an external quantum efficiency (the spectrally resolved ratio of collected charge carriers to incident photons) that peaked at 114 ± 1% in the best device measured. The associated internal quantum efficiency (corrected for reflection and absorption losses) was 130%. We compare our results with transient absorption measurements of MEG in isolated PbSe QDs and find reasonable agreement. Our findings demonstrate that MEG charge carriers can be collected in suitably designed QD solar cells, providing ample incentive to better understand MEG within isolated and coupled QDs as a research path to enhancing the efficiency of solar light harvesting technologies.
Femtosecond resolution electron scattering techniques are applied to resolve the first atomic-scale steps following absorption of a photon in the prototypical hybrid perovskite methylammonium lead iodide. Following above-gap photoexcitation, we directly resolve the transfer of energy from hot carriers to the lattice by recording changes in the mean square atomic displacements on 10-ps time scales. Measurements of the time-dependent pair distribution function show an unexpected broadening of the iodine-iodine correlation function while preserving the Pb-I distance. This indicates the formation of a rotationally disordered halide octahedral structure developing on picosecond time scales. This work shows the important role of light-induced structural deformations within the inorganic sublattice in elucidating the unique optoelectronic functionality exhibited by hybrid perovskites and provides new understanding of hot carrier-lattice interactions, which fundamentally determine solar cell efficiencies.
Cosmic rays are particles (mostly protons) accelerated to relativistic speeds. Despite wide agreement that supernova remnants (SNRs) are the sources of galactic cosmic rays, unequivocal evidence for the acceleration of protons in these objects is still lacking. When accelerated protons encounter interstellar material, they produce neutral pions, which in turn decay into gamma rays. This offers a compelling way to detect the acceleration sites of protons. The identification of pion-decay gamma rays has been difficult because high-energy electrons also produce gamma rays via bremsstrahlung and inverse Compton scattering. We detected the characteristic pion-decay feature in the gamma-ray spectra of two SNRs, IC 443 and W44, with the Fermi Large Area Telescope. This detection provides direct evidence that cosmic-ray protons are accelerated in SNRs.
- Proceedings of the National Academy of Sciences of the United States of America
- Published over 5 years ago
The precise knowledge of one of two complementary experimental outcomes prevents us from obtaining complete information about the other one. This formulation of Niels Bohr’s principle of complementarity when applied to the paradigm of wave-particle dualism–that is, to Young’s double-slit experiment–implies that the information about the slit through which a quantum particle has passed erases interference. In the present paper we report a double-slit experiment using two photons created by spontaneous parametric down-conversion where we observe interference in the signal photon despite the fact that we have located it in one of the slits due to its entanglement with the idler photon. This surprising aspect of complementarity comes to light by our special choice of the TEM(01) pump mode. According to quantum field theory the signal photon is then in a coherent superposition of two distinct wave vectors giving rise to interference fringes analogous to two mechanical slits.
Quantum systems exhibit particle- or wavelike behavior depending on the experimental apparatus they are confronted by. This wave-particle duality is at the heart of quantum mechanics. Its paradoxical nature is best captured in the delayed-choice thought experiment, in which a photon is forced to choose a behavior before the observer decides what to measure. Here, we report on a quantum delayed-choice experiment in which both particle and wave behaviors are investigated simultaneously. The genuinely quantum nature of the photon’s behavior is certified via nonlocality, which here replaces the delayed choice of the observer in the original experiment. We observed strong nonlocal correlations, which show that the photon must simultaneously behave both as a particle and as a wave.
Vertical arrays of ZnO nanowires can decouple light absorption from carrier collection in PbS quantum dot solar cells and increase power conversion efficiencies by 35%. The resulting ordered bulk heterojunction devices achieve short-circuit current densities in excess of 20 mA cm(-2) and efficiencies of up to 4.9%.
The energy costs associated with separating tightly bound excitons (photoinduced electron-hole pairs) and extracting free charges from highly disordered low-mobility networks represent fundamental losses for many low-cost photovoltaic technologies. We report a low-cost, solution-processable solar cell, based on a highly crystalline perovskite absorber with intense visible to near-infrared absorptivity, that has a power conversion efficiency of 10.9% in a single-junction device under simulated full sunlight. This “meso-superstructured solar cell” exhibits exceptionally few fundamental energy losses; it can generate open-circuit photovoltages of more than 1.1 volts, despite the relatively narrow absorber band gap of 1.55 electron volts. The functionality arises from the use of mesoporous alumina as an inert scaffold that structures the absorber and forces electrons to reside in and be transported through the perovskite.
In contrast to pristine zinc phthalocyanine (1), zinc phthalocyanine based oPPV-oligomers (2-4) of different chain lengths interact tightly and reversibly with graphite, affording stable and finely dispersed suspensions of mono- to few-layer graphene-nanographene (NG)-that are photoactive. The p-type character of the oPPV backbones and the increasing length of the oPPV backbones facilitate the overall π-π interactions with the graphene layers. In NG/2, NG/3, and NG/4 hybrids, strong electronic coupling between the individual components gives rise to charge transfer from the photoexcited zinc phthalocyanines to NG to form hundreds of picoseconds lived charge transfer states. The resulting features, namely photo- and redoxactivity, serve as incentives to construct and to test novel solar cells. Solar cells made out of NG/4 feature stable and repeatable photocurrent generation during several ‘on-off’ cycles of illumination with monochromatic IPCE values of around 1%.