Quantum information, a field in which great advances have been made in the past decades, now presents opportunities for advanced chemistry. One roadblock to progress, especially for experimental ...chemical science, is that new concepts and technical definitions need to be learned. In this paper, we review some basic, but sometimes misunderstood, concepts of quantum information based on the mathematical formulation of quantum mechanics that will be useful for chemists interested in discovering ways that chemistry can contribute to the quantum information field. We cover topics including qubits and their density matrix formalism, quantum measurement as a quantum operation, information theory, and entanglement. We focus on the difference between the concepts in the quantum context and the classic context. We also discuss the relation and distinction among entanglement, correlation, and coherence. We aim to clarify the rigorous definition of these concepts and then indicate some examples in physical chemistry.
Waveplates are widely used in photonics to control the polarization of light1,2. Often, they are fabricated from birefringent crystals that have different refractive indices along and normal to the ...crystal axis. Similar optical components are found in the natural world, including the eyes of mantis shrimp3,4 and the iridescence of giant clams5, fish6 and plants7. Optical retardation in biology relies on sophisticated self-assembly, whereas man-made systems comprise multiple-layered materials8–11. Here we report a discovery that bridges these two design principles. We observe wideband achromatic retardation in the visible and near-infrared (532–800 nm) regions for Cs4PbBr6 perovskite crystals embedded with CsPbBr3 nanocrystals. We explain our observations as matched dispersions of the refractive indices of the ordinary and extraordinary rays caused by the ordered embedding of the nanocrystals in the host. The wideband performance and ease of fabrication of these perovskite materials are attractive for future applications.Perovskite crystals of Cs4PbBr6 embedded with CsPbBr3 nanocrystals are shown to act as wideband, achromatic waveplates in the visible and near-infrared regions.
Pyrene is an exemplary conjugated organic chromophore with a strong propensity for self-association through an excited-state process known as excimer formation. Pyrene “excimers” and molecular ...“excimers” more generally are strongly avoided in some applications, such as in light harvesting, yet have found widespread use in others, such as in sensing and structure determination. Despite this disparate view and despite their widespread use, a fundamental understanding of the structure and dynamics of these collective excitations remains outstanding. In this work, we shed key insights into the nature of excimer formation in crystalline pyrene. We developed a flash precipitation procedure incorporating a polymer additive that enabled us to prepare aqueous suspensions of crystalline pyrene nanoparticles. We provide evidence that the molecular-level packing in the nanoparticles is equivalent to the equilibrium packing of the single crystal and show that excimer formation is the primary excited-state decay pathway. We find that excimer formation in the crystalline pyrene nanoparticles occurs in two stages on a picosecond time scale and suggest that intermolecular structural dynamics are largely responsible for the observed two-stage dynamics. We discuss an exciton theory description of molecular “excimers” and provide insights into their mechanism of formation, which we argue is best viewed simply as the relaxation of a singlet exciton into an excimer geometry.
Essential Biodiversity Variables Pereira, H. M.; Ferrier, S.; Walters, M. ...
Science (American Association for the Advancement of Science),
01/2013, Letnik:
339, Številka:
6117
Journal Article
Recenzirano
Reducing the rate of biodiversity loss and averting dangerous biodiversity change are international goals, reasserted by the Aichi Targets for 2020 by Parties to the United Nations (UN) Convention on ...Biological Diversity (CBD) after failure to meet the 2010 target (1, 2). However, there is no global, harmonized observation system for delivering regular, timely data on biodiversity change (3). With the first plenary meeting of the Intergovernmental Science-Policy Platform on Biodiversity and Ecosystem Services (IPBES) soon under way, partners from the Group on Earth Observations Biodiversity Observation Network (GEO BON) (4) are developing-and seeking consensus around-Essential Biodiversity Variables (EBVs) that could form the basis of monitoring programs worldwide.
Electronic coherence has attracted considerable attention for its possible role in dynamical processes in molecular systems. However, its detection is challenged by inhomogeneous line broadening and ...interference with vibrational coherences. In particular, reports of 'persistent' coherent exciton superpositions at room temperature remain controversial, as the related transitions give typically shorter optical dephasing times of about 10-20 fs. To rationalize these reported long-lived coherences, several models have been proposed, involving strong correlation in the mechanisms of decoherence or that electronic coherences may be sustained by resonant vibrational modes. Here we report a decisive example of electronic coherence occurring in a chemical system in a 'warm and wet' (room-temperature solution) environment, colloidal semiconductor nanoplatelets, where details are not obscured by vibrational coherences nor ensemble dephasing. Comparing the exciton and optical coherence times evidences a partial correlation of fluctuations underlying dephasing and allows us to elucidate decoherence mechanisms occurring in these samples.
The past decade has seen rapid advances in our understanding of how coherent and vibronic phenomena in biological photosynthetic systems aid in the efficient transport of energy from light-harvesting ...antennas to photosynthetic reaction centres. Such coherence effects suggest strategies to increase transport lengths even in the presence of structural disorder. Here we explore how these principles could be exploited in making improved solar cells. We investigate in depth the case of organic materials, systems in which energy and charge transport stand to be improved by overcoming challenges that arise from the effects of static and dynamic disorder - structural and energetic - and from inherently strong electron-vibration couplings. We discuss how solar-cell device architectures can evolve to use coherence-exploiting materials, and we speculate as to the prospects for a coherent energy conversion system. We conclude with a survey of the impacts of coherence and bioinspiration on diverse solar-energy harvesting solutions, including artificial photosynthetic systems.
The conversion of photoexcitations into charge carriers in organic solar cells is facilitated by the dissociation of excitons at the donor/acceptor interface. The ultrafast timescale of charge ...separation demands sophisticated theoretical models and raises questions about the role of coherence in the charge-transfer mechanism. Here, we apply two-dimensional electronic spectroscopy to study the electron transfer process in poly(3-hexylthiophene)/PCBM (P3HT/PCBM) blends. We report dynamics maps showing the pathways of charge transfer that clearly expose the significance of hot electron transfer. During this ultrafast electron transfer, vibrational coherence is directly transferred from the P3HT exciton to the P3HT hole polaron in the crystalline domain. This result reveals that the exciton converts to a hole with a similar spatial extent on a timescale far exceeding other photophysical dynamics including vibrational relaxation.
The influence of fast vibrations on energy transfer and conversion in natural molecular aggregates is an issue of central interest. This article shows the important role of high-energy quantized ...vibrations and their non-equilibrium dynamics for energy transfer in photosynthetic systems with highly localized excitonic states. We consider the cryptophyte antennae protein phycoerythrin 545 and show that coupling to quantized vibrations, which are quasi-resonant with excitonic transitions is fundamental for biological function as it generates non-cascaded transport with rapid and wider spatial distribution of excitation energy. Our work also indicates that the non-equilibrium dynamics of such vibrations can manifest itself in ultrafast beating of both excitonic populations and coherences at room temperature, with time scales in agreement with those reported in experiments. Moreover, we show that mechanisms supporting coherent excitonic dynamics assist coupling to selected modes that channel energy to preferential sites in the complex. We therefore argue that, in the presence of strong coupling between electronic excitations and quantized vibrations, a concrete and important advantage of quantum coherent dynamics is precisely to tune resonances that promote fast and effective energy distribution.
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