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A single crystal growth method for low solubility polycyclic aromatic substrates based on competitive host–guest equilibria is developed.

 

Terpenoids constitute the largest class of plant primary and secondary metabolites with a broad range of biological and ecological functions. They are synthesized from isopentenyl diphosphate and dimethylallyl diphosphate, which in plastids are condensed by geranylgeranyl diphosphate synthases (GGPPSs) to produce GGPP (C20) for diterpene biosynthesis and by geranyl diphosphate synthases (GPPSs) to form GPP (C10) for monoterpene production. Depending on the plant species, unlike homomeric GGPPSs, GPPSs exist as homo- and heteromers, the latter of which contain catalytically inactive GGPPS-homologous small subunits (SSUs) that can interact with GGPPSs. By combining phylogenetic analysis with functional characterization of GGPPS homologs from a wide range of photosynthetic organisms, we investigated how different GPPS architectures have evolved within the GGPPS protein family. Our results reveal that GGPPS gene family expansion and functional divergence began early in nonvascular plants, and that independent parallel evolutionary processes gave rise to homomeric and heteromeric GPPSs. By site-directed mutagenesis and molecular dynamics simulations, we also discovered that Leu-Val/Val-Ala pairs of amino acid residues were pivotal in the functional divergence of homomeric GPPSs and GGPPSs. Overall, our study elucidated an evolutionary path for the formation of GPPSs with different architectures from GGPPSs and uncovered the molecular mechanisms involved in this differentiation.

 

Spontaneous parametric down conversion (PDC), in the perturbative limit, can be considered as a probabilistic splitting of one input photon into two output photons. Conversely, sum-frequency generation (SFG) implements the reverse process of combining two input photons into one. Here we show that a single-photon projective measurement in the temporal-mode basis of the output photon of a two-photon SFG process affects a generalized measurement on the input two-photon state. We describe the positive operator-valued measure (POVM) associated with such a measurement and show that its elements are proportional to the two-photon states produced by the time-reversed PDC process. Such a detection acts as a joint measurement on two photons and is thus an important component of many quantum information processing protocols relying on photonic entanglement. Using the retrodictive approach, we analyze the properties of the two-photon POVM that are relevant for quantum protocols exploiting two-photon states and measurements. 

We present a theoretical proof that the “quantum enhancement” of two-photon absorption, thought to be a means to improve molecular spectroscopy and imaging, is tightly bounded by the physics of photonic entanglement and nonlinear response.

 

The theory of sum-frequency generation (SFG) as a two-photon measurement process is used to infer the role of two-photon entanglement in this process, and an experimental setup and preliminary data are presented as a way towards quantifying the dependence of SFG on entanglement.

 

Quantum entanglement plays a prominent role in both foundational physics and emerging quantum technologies. Light is especially promising as a platform for experimental realizations of high-dimensional entanglement, for which the time-frequency degree of freedom provides a natural encoding. Here, we propose and demonstrate a technique to determine the full quantum state of a pair of photons entangled in the time-frequency domain. Our approach, based on spectral shearing interferometry, is entirely self-referenced. To test our system, we measure a photon-pair source with nonlocal spectral phase that results in entanglement between the photons, in which the time when either photon is detected is correlated with the frequency of the other photon. The results demonstrate an effective new tool for exploring the temporal and spectral characteristics of multipartite quantum systems exhibiting high-dimensional entanglement.

 

Controlling the temporal mode shape of quantum light pulses has wide ranging application to quantum information science and technology. Techniques have been developed to control the bandwidth, allow shifting in the time and frequency domains, and perform mode-selective beam-splitter-like transformations. However, there is no present scheme to perform targeted multimode unitary transformations on temporal modes. Here we present a practical approach to realize general transformations for temporal modes. We show theoretically that any unitary transformation on temporal modes can be performed using a series of phase operations in the time and frequency domains. Numerical simulations show that several key transformations on temporal modes can be performed with greater than 95% fidelity using experimentally feasible specifications.