抗原变异可使得多种致病微生物易于逃避宿主免疫应答。表达在感染红细胞表面的恶性疟原虫红细胞表面蛋白1（PfPMP1）与感染红细胞、内皮细胞、树突状细胞以及胎盘的单个或多个受体作用，在黏附及免疫逃避中起关键的作用。每个单倍体基因组var基因家族编码约60种成员，通过启动转录不同的var基因变异体为抗原变异提供了分子基础。

疟原虫var基因转换速率变化导致抗原变异[英]／Paul H, Robert P, Christodoulou Z, et al//Proc Natl Acad Sci U S A

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Principles Of Fluorescence Spectroscopy

Colloidal nanoparticles are being intensely pursued in current nanoscience research. Nanochemists are often frustrated by the well-known fact that no two nanoparticles are the same, which precludes the deep understanding of many fundamental properties of colloidal nanoparticles in which the total structures (core plus surface) must be known. Therefore, controlling nanoparticles with atomic precision and solving their total structures have long been major dreams for nanochemists. Recently, these goals are partially fulfilled in the case of gold nanoparticles, at least in the ultrasmall size regime (1–3 nm in diameter, often called nanoclusters). This review summarizes the major progress in the field, including the principles that permit atomically precise synthesis, new types of atomic structures, and unique physical and chemical properties of atomically precise nanoparticles, as well as exciting opportunities for nanochemists to understand very fundamental science of colloidal nanoparticles (such as the s...

Atomically Precise Colloidal Metal Nanoclusters and Nanoparticles: Fundamentals and Opportunities

Solar energy is an alternative, sustainable energy source for mankind. Finding a convenient way to convert sunlight energy into chemical energy is a key step towards realizing large-scale solar energy utilization. Owing to their structural regularity and synthetic tunability, metal–organic frameworks (MOFs) provide an interesting platform to hierarchically organize light-harvesting antennae and catalytic centers to achieve solar energy conversion. Such photo-driven catalytic processes not only play a critical role in the solar to chemical energy conversion scheme, but also provide a novel methodology for the synthesis of fine chemicals. In this review, we summarize the fundamental principles of energy transfer and photocatalysis and provide an overview of the latest progress in energy transfer, light-harvesting, photocatalytic proton and CO2 reduction, and water oxidation using MOFs. The applications of MOFs in organic photocatalysis and degradation of model organic pollutants are also discussed.

Metal–organic frameworks for artificial photosynthesis and photocatalysis

One of the most intriguing and most studied features of photosynthesis is the exquisite efficiency with which energy can be transferred within photosynthetic complexes. A new spectroscopic study confirms earlier hints that quantum effects might be at play, by directly revealing quantum-coherent sharing of electronic excitation across 5-nm-wide photosynthetic proteins from Chroomonas CCMP270 marine algae at room temperature. The observation suggests that distant units within the proteins are 'wired' together by quantum-coherence to enhance light-harvesting efficiency. Photosynthesis makes use of sunlight to convert carbon dioxide into useful biomass and is vital for life on Earth. Crucial components for the photosynthetic process are antenna proteins, which absorb light and transmit the resultant excitation energy between molecules to a reaction centre. The efficiency of these electronic energy transfers has inspired much work on antenna proteins isolated from photosynthetic organisms to uncover the basic mechanisms at play1,2,3,4,5. Intriguingly, recent work has documented6,7,8 that light-absorbing molecules in some photosynthetic proteins capture and transfer energy according to quantum-mechanical probability laws instead of classical laws9 at temperatures up to 180 K. This contrasts with the long-held view that long-range quantum coherence between molecules cannot be sustained in complex biological systems, even at low temperatures. Here we present two-dimensional photon echo spectroscopy10,11,12,13 measurements on two evolutionarily related light-harvesting proteins isolated from marine cryptophyte algae, which reveal exceptionally long-lasting excitation oscillations with distinct correlations and anti-correlations even at ambient temperature. These observations provide compelling evidence for quantum-coherent sharing of electronic excitation across the 5-nm-wide proteins under biologically relevant conditions, suggesting that distant molecules within the photosynthetic proteins are ‘wired’ together by quantum coherence for more efficient light-harvesting in cryptophyte marine algae.

Coherently wired light-harvesting in photosynthetic marine algae at ambient temperature

A variety of two-dimensional electronic spectroscopy experiments on natural light-harvesting complexes reveal inter-chromophore coupling and monitor ultrafast dynamics, furthering understanding of the way these proteins function and the underlying design principles of photosynthesis

Two-dimensional Electronic Spectroscopy of Photosynthetic Light-Harvesting Complexes

The phycobilisome is the primary light-harvesting antenna in cyanobacterial and red algal oxygenic photosynthesis. It maintains near-unity efficiency of energy transfer to reaction centers despite relying on slow exciton hopping along a relatively sparse network of highly fluorescent phycobilin chromophores. How the complex maintains this high efficiency remains unexplained. Using a two-dimensional electronic spectroscopy polarization scheme that enhances energy transfer features, we directly watch energy flow in the phycobilisome complex of Synechocystis sp. PCC 6803 from the outer phycocyanin rods to the allophycocyanin core. The observed downhill flow of energy, previously hidden within congested spectra, is faster than timescales predicted by Förster hopping along single rod chromophores. We attribute the fast, 8 ps energy transfer to interactions between rod-core linker proteins and terminal rod chromophores, which facilitate unidirectionally downhill energy flow to the core. This mechanism drives the high energy transfer efficiency in the phycobilisome and suggests that linker protein–chromophore interactions have likely evolved to shape its energetic landscape.

https://pubs.acs.org/doi/pdf/10.1021/jacs.3c01799

Phycobilisome’s Exciton Transfer Efficiency Relies on an Energetic Funnel Driven by Chromophore–Linker Protein Interactions

We present a chiral two-dimensional mapping of light harvesting complex 2. This methodology allows us to follow femtosecond changes in the chirality of the electronic structure, providing detailed insights into the excitation energy transfer events.

Probing Delocalization in Photosynthetic Antenna Complexes with Femtosecond Chiral Two-Dimensional Spectroscopy

The B800 band of the reaction center complex of Rhodobacter sphaeroides has been probed with two-dimensional Fourier transform electronic spectroscopy using 40 fs pulses and evidence for coupling within the band will be presented.

Gregory S. Engel

Papers

Two-dimensional Electronic Spectroscopy of Photosynthetic Light-Harvesting Complexes

Phycobilisome’s Exciton Transfer Efficiency Relies on an Energetic Funnel Driven by Chromophore–Linker Protein Interactions

Probing Delocalization in Photosynthetic Antenna Complexes with Femtosecond Chiral Two-Dimensional Spectroscopy

2D Fourier Transform Electronic Spectroscopy of Photosynthetic Reaction Centers: Mapping coupling in the B band