Phototheranostics represents a promising direction for modern precision medicine, which has recently attracted great research interest from multidisciplinary research areas. Organic optical agents ...including small molecular fluorophores, semiconducting/conjugated polymers, aggregation-induced emission luminogens, etc. with tuneable photophysical properties, high biosafety and biocompatibility, facile processability and ease of functionalization have delivered encouraging performance in disease phototheranostics. This review summarizes the recent progress of organic phototheranostic agents with an emphasis on the main strategies to manipulate the three excitation energy dissipation pathways, namely, radiative decay, thermal deactivation, and intersystem crossing, with the assistance of a Jablonski diagram, which particularly showcases how the Jablonski diagram has been guiding the design of organic agents from molecule to aggregate levels to promote the disease phototheranostic outcomes. Molecular design and nanoengineering strategies to modulate photophysical processes of organic optical agents to convert the absorbed photons into fluorescent/phosphorescent/photoacoustic signals and/or photodynamic/photothermal curing effects for improved disease phototheranostics are elaborated. Noteworthily, adaptive phototheranostics with activatable and transformable functions on demand, and regulation of excitation such as chemiexcitation to promote the phototheranostic efficacies are also included. A brief summary with the discussion of current challenges and future perspectives in this research field is further presented.
J-aggregation is an efficient strategy for the development of fluorescent imaging agents in the second near-infrared window. However, the design of the second near-infrared fluorescent J-aggregates ...is challenging due to the lack of suitable J-aggregation dyes. Herein, we report meso-2.2paracyclophanyl-3,5-bis-N,N-dimethylaminostyrl BODIPY (PCP-BDP2) as an example of BODIPY dye with J-aggregation induced the second near-infrared fluorescence. PCP-BDP2 shows an emission maximum at 1010 nm in the J-aggregation state. Mechanism studies reveal that the steric and conjugation effect of the PCP group on the BODIPY play key roles in the J-aggregation behavior and photophysical properties tuning. Notably, PCP-BDP2 J-aggregates can be utilized for lymph node imaging and fluorescence-guided surgery in the nude mouse, which demonstrates their potential clinical application. This study demonstrates BODIPY dye as an alternate J-aggregation platform for developing the second near-infrared imaging agents.
Polyhydroxyalkanoates (PHAs) are a diverse family of biopolyesters synthesized by many natural or engineered bacteria. Synthetic biology and DNA-editing approaches have been adopted to engineer cells ...for more efficient PHA production. Recent advances in synthetic biology applied to improve PHA biosynthesis include ribosome-binding site (RBS) optimization, promoter engineering, chromosomal integration, cell morphology engineering, cell growth behavior reprograming, and downstream processing. More importantly, the genome-editing tool clustered regularly interspaced short palindromic repeats (CRISPR)/CRISPR-associated protein 9 (Cas9) has been applied to optimize the PHA synthetic pathway, regulate PHA synthesis-related metabolic flux, and control cell shapes in model organisms, such as Escherichia coli, and non-model organisms, such as Halomonas. These synthetic biology methods and genome-editing tools contribute to controllable PHA molecular weights and compositions, enhanced PHA accumulation, and easy downstream processing.
The bioplastic PHA, which features biodegradability, biocompatibility, and thermoprocessibility, is moving toward low-cost microbial production to replace nondegradable petrochemical plastics.Wild-type or weakly engineered bacteria are insufficient to meet demands for improved PHA structures and low production cost.Synthetic biology and genome-editing approaches can promote PHA synthesis, enlarge cells for more PHA storage, control shape changes, accelerate growth, aid the co-production of multiple products, direct flux toward final products, and make product recovery more convenient.Optimized promoters and RBSs increase the expression of PHA synthesis genes.CRISPR interference and CRISPR/Cas9 are useful for downregulating the expression of multiple genes simultaneously, allowing more flux to be directed to PHA synthesis in an optimized strain.
Persistent luminescence without excitation light and tissue autofluorescence interference holds great promise for biological applications, but is limited by available materials with long‐wavelength ...emission and excellent clinical potential. Here, we report that porphyrin derivatives can emit near‐infrared persistent luminescence over 60 min after cessation of excitation light or on interaction with peroxynitrite. A plausible mechanism of the successive oxidation of vinylene bonds was demonstrated. A supramolecular probe with a β‐sheet structure was constructed to enhance the tumor targeting ability and the photoacoustic and persistent luminescence signals. Such probes featuring light‐triggered function transformation from photoacoustic imaging to persistent luminescence imaging permit advanced image‐guided cancer surgery. Furthermore, peroxynitrite‐activated persistent luminescence of the supramolecular probe also enables rapid and precise screening of immunogenic cell death drugs.
Porphyrin derivatives that can emit near‐infrared persistent luminescence (PL) over 60 min are reported and a mechanism for the phenomenon is proposed. The derivatives are used to synthesize supramolecular probes with peroxynitrite‐activated PL and light‐triggered imaging‐modality transformation characteristics that permit improved biological uses.
The emerged strategy of entropy engineering provides new ideas for realizing high‐performance thermoelectric materials, but it is still much unresolved how to achieve delicate trade‐off between the ...carrier mobility mH and the lattice thermal conductivity κph in taking advantage of configurational entropy ΔS. Herein, the significant advances of ultralow κph yet decent mH in a new medium‐entropy system of well‐designed (Pb, Ge, Sb, Cd) co‐alloyed SnTe is reported. Moreover, the co‐alloying also optimizes the carrier concentration nH and promotes the valence band convergence, thereby yielding an excellent Seebeck coefficient and compensating for decreased electrical conductivity. Consequently, a high peak ZT of 1.5 at 800 K, a record average ZT of 0.84 (300−800 K), and a remarkable Vickers hardness of 134 HV are concurrently attained in Cd0.02(Sn0.59Pb0.15Ge0.2Sb0.06)0.98Te. Benefiting from the synergistically increased ZT and mechanical strength, the fabricated 17‐couple SnTe‐based thermoelectric module exhibits a competitive conversion efficiency of 6.3% at ΔT = 350 °C. This study not only provides a paradigm of the medium‐entropy design for thermoelectric materials but also puts forward an innovative scheme for low‐grade heat harvest by SnTe‐based TE module.
The medium‐entropy design proposes a feasible solution to crucial issue of entropy engineering, and thus realizes ultralow κph yet decent mH successfully. Consequently, a high ZTmax of 1.5 at 800 K, a record ZTave of 0.84 (300−800 K), and competitive conversion efficiency of 6.3% (ΔT = 350 °C) are achieved for low‐grade heat harvest.
The gold standard for diagnosing sleep disorders is polysomnography, which generates extensive data about biophysical changes occurring during sleep. We developed the National Sleep Research Resource ...(NSRR), a comprehensive system for sharing sleep data. The NSRR embodies elements of a data commons aimed at accelerating research to address critical questions about the impact of sleep disorders on important health outcomes.
We used a metadata-guided approach, with a set of common sleep-specific terms enforcing uniform semantic interpretation of data elements across three main components: (1) annotated datasets; (2) user interfaces for accessing data; and (3) computational tools for the analysis of polysomnography recordings. We incorporated the process for managing dataset-specific data use agreements, evidence of Institutional Review Board review, and the corresponding access control in the NSRR web portal. The metadata-guided approach facilitates structural and semantic interoperability, ultimately leading to enhanced data reusability and scientific rigor.
The authors curated and deposited retrospective data from 10 large, NIH-funded sleep cohort studies, including several from the Trans-Omics for Precision Medicine (TOPMed) program, into the NSRR. The NSRR currently contains data on 26 808 subjects and 31 166 signal files in European Data Format. Launched in April 2014, over 3000 registered users have downloaded over 130 terabytes of data.
The NSRR offers a use case and an example for creating a full-fledged data commons. It provides a single point of access to analysis-ready physiological signals from polysomnography obtained from multiple sources, and a wide variety of clinical data to facilitate sleep research.
Nonlocal self-similarity of images has attracted considerable interest in the field of image processing and has led to several state-of-the-art image denoising algorithms, such as block matching and ...3-D, principal component analysis with local pixel grouping, patch-based locally optimal wiener, and spatially adaptive iterative singular-value thresholding. In this paper, we propose a computationally simple denoising algorithm using the nonlocal self-similarity and the low-rank approximation (LRA). The proposed method consists of three basic steps. First, our method classifies similar image patches by the block-matching technique to form the similar patch groups, which results in the similar patch groups to be low rank. Next, each group of similar patches is factorized by singular value decomposition (SVD) and estimated by taking only a few largest singular values and corresponding singular vectors. Finally, an initial denoised image is generated by aggregating all processed patches. For low-rank matrices, SVD can provide the optimal energy compaction in the least square sense. The proposed method exploits the optimal energy compaction property of SVD to lead an LRA of similar patch groups. Unlike other SVD-based methods, the LRA in SVD domain avoids learning the local basis for representing image patches, which usually is computationally expensive. The experimental results demonstrate that the proposed method can effectively reduce noise and be competitive with the current state-of-the-art denoising algorithms in terms of both quantitative metrics and subjective visual quality.
Abstract
Ectoine, a compatible solute synthesized by many halophiles for hypersalinity resistance, has been successfully produced by metabolically engineered
Halomonas bluephagenesis
, which is a ...bioplastic poly(3-hydroxybutyrate) producer allowing open unsterile and continuous conditions. Here we report a de novo synthesis pathway for ectoine constructed into the chromosome of
H. bluephagenesis
utilizing two inducible systems, which serve to fine-tune the transcription levels of three clusters related to ectoine synthesis, including
ectABC
,
lysC
and
asd
based on a GFP-mediated transcriptional tuning approach. Combined with bypasses deletion, the resulting recombinant
H. bluephagenesis
TD-ADEL-58 is able to produce 28 g L
−1
ectoine during a 28 h fed-batch growth process. Co-production of ectoine and PHB is achieved to 8 g L
−1
ectoine and 32 g L
−1
dry cell mass containing 75% PHB after a 44 h growth.
H. bluephagenesis
demonstrates to be a suitable co-production chassis for polyhydroxyalkanoates and non-polymer chemicals such as ectoine.
Development of the powerful building block is of great significance to construct materials with advanced properties. Herein, for the first time, a triazole‐based luminescent core with balanced twist ...and conjugation is reported, which is explored to construct a D‐A near‐infrared (NIR) aggregation‐induced emission luminogens (TPT‐DCM) with high molar extinction coefficient, good brightness and excellent reactive oxygen species generation rate. These features enable it to function as a nanoprobe with ultralong NIR afterglow luminescence (up to 20 days) and ultrahigh tumor‐to‐liver signal ratio (up to 187) for in vivo deep‐tissue afterglow imaging (with depth reaching 1.6 cm), in combination with chemiluminescence resonance energy transfer aided by active Schaap's dioxetane. Moreover, thanks to the excellent properties of the nanoprobe, the afterglow imaging‐guided surgery navigation can be successfully conduced to remove the tumors especially with tiny size of < 1 mm. This is particularly useful to eliminate tumor residuals and prevent the cancer recurrence after surgery.
Robust trizole‐based luminescent core with balanced twist and conjugation is reported to construct near‐infrared (NIR) aggregation‐induced emission luminogens (TPT‐DCM) and ultralong NIR afterglow nanoprobe, which shows great potential for high‐contrast tumor imaging and afterglow imaging‐guided surgery navigation.
The good co‐existence of midgap state and valence band degeneracy is realized in Bi‐alloyed GeTe through the In‐Cd codoping to play different but complementary roles in the valence band structure ...modification. In doping induces midgap state and results in a considerably improved Seebeck coefficient near room temperature, while Cd doping significantly increases the Seebeck coefficient in the mid‐high temperature region by promoting the valence band convergence. The synergistic effects obviously increase the density of state effective mass from 1.39 to 2.65 m0, and the corresponding carrier mobility still reaches 34.3 cm2 V−1 s−1 at room temperature. Moreover, the Bi‐In‐Cd co‐alloying introduces various phonon scattering centers including nanoprecipitates and strain field fluctuations and suppresses the lattice thermal conductivity to a rather low value of 0.56 W m−1 K−1 at 600 K. As a result, the Ge0.89Bi0.06In0.01Cd0.04Te sample obtains excellent thermoelectric properties of zTmax ≈2.12 at 650 K and zTavg ≈1.43 between 300 and 773 K. This study illustrates that the thermoelectric performance of GeTe can be optimized in a wide temperature range through the synergy of midgap state and valence band convergence.
It is revealed that the good coexistence of midgap state and band convergence in GeTe improves the thermoelectric performance over a very broad temperature range. Since the high md∗$m_d^ * $ is obtained and the κl is reduced, the thermoelectric performance of GeTe is significantly improved, leading to a high zTmax of 2.12 at 650 K and a greatly improved zTavg of 1.43 between 300 and 773 K.
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