Unveiling the synthesis of aromatic compounds in sauce-flavor Daqu from the functional microorganisms to enzymes.

Aromatic compounds serve as the primary source of floral and fruity aromas in sauce-flavor (Maotai flavor) baijiu, constituting the skeleton components of its flavor profile. Nevertheless, the formation mechanism of these compounds and key aroma-producing enzymes in sauce-flavor Daqu (fermentation agent, SFD) remain elusive. Here, we combined metagenomics, metaproteomics, metabolomics, and key enzyme activity to verify the biosynthesis pathway of aromatic compounds and to identify key enzymes, genes, and characteristic microorganisms in SFD. The results showed that the later period of fermentation was critical for the generation of aromatic compounds in SFD. In-situ verification was conducted on the potential key enzymes and profiles in various metabolites, providing comprehensive evidence for the main synthetic pathways of aromatic compounds in SFD. Notably, our results showed that primary amine oxidase (PrAO) and aldehyde dehydrogenase (ALDH) emerged as two key enzymes promoting aromatic compound synthesis. Additionally, two potential key functional genes regulating aromatics generation were identified during SFD fermentation through correlation analysis between proteins and relevant metabolites, coupled with in vitro amplification test. Furthermore, original functional strains (Aspergillus flavus-C10 and Aspergillus niger-IN2) exhibiting high PrAO and ALDH production were successfully isolated from SFD, thus validating the results of metagenomics and metaproteomics analyses. This study comprehensively elucidates the pathway of aromatic compound formation in SFD at the genetic, proteomic, enzymatic, and metabolomic levels, providing new ideas for the investigation of key flavor substances in baijiu. Additionally, these findings offer valuable insights into the regulatory mechanisms of aromatic compounds generation.

Effects of pickle brine and glycine addition on biogenic amine production in pickle fermentation.

This study investigated the effects of different pickle brines and glycine additions on biogenic amine formation in pickle fermentation. The results showed that the brines with higher biogenic amine content led to the production of more biogenic amines in the simulated pickle fermentation system. This was related to the abundance of biogenic amine-producing microorganisms in the microbial communities of the brines. Metagenome analysis of the brines and metatranscriptome analysis of the fermentation systems showed that putrescine was primarily from Lactobacillus, Oenococcus, and Pichia, while histamine and tyramine were primarily from Lactobacillus and Tetragenococcus. Addition of glycine significantly reduced the accumulation of biogenic amines in the simulated pickle fermentation system by as much as 70 %. The addition of glycine had no inhibitory effect on the amine-producing microorganisms, but it down-regulated the transcription levels of the genes for enzymes related to putrescine synthesis in Pichia, Lactobacillus, and Oenococcus, as well as the histidine decarboxylase genes in Lactobacillus and Tetragenococcus. Catalytic reaction assay using crude solutions of amino acid decarboxylase extracted from Lactobacillus brevis showed that the addition of glycine inhibited 45 %-55 % of ornithine decarboxylase and tyrosine decarboxylase activities. This study may provide a reference for the study and control of the mechanism of biogenic amine formation in pickle fermentation.

Exploring the regulated effects of solid-state fortified Jiuqu and liquid-state fortified agent on Chinese Baijiu brewing.

Zaopei is the direct source of Chinese liquor (Baijiu). Adding functional strains to Zaopei is a potential strategy to regulate Baijiu brewing, mainly including the two ways of solid-state fortified Jiuqu (SFJ) and liquid-state fortified agent (LFA). Here, to explore their regulated details, the response patterns of Zaopei microecosystem and the changes in the product features were comprehensively investigated. The results showed that SFJ more positively changed the physicochemical properties of Zaopei and improved its ester content, from 978.57 mg/kg to 1078.63 mg/kg over the fermentation of 30 days, while LFA decreased the content of esters, alcohols, and acids. Microbial analysis revealed that SFJ significantly increased Saccharomycopsis and Aspergillus from the start of fermentation and induced a positive interaction cluster driven by the added functional Paenibacillus, while LFA exhibited a community structure near that of the original microecosystem and led to a simpler network with the reduced microbial nodes and correlations. Metabolism analysis found that both SFJ and LFA weakened the flavor-producing metabolism by suppressing some key enzyme pathways, such as EC 3.2.1.51, EC 4.2.1.47, EC 1.1.1.27, EC 1.1.1.22, EC 1.5.1.10, EC 1.14.11.12. As a result, SFJ improved the raw liquor yield by 28.5 % and endowed the final product with a more fragrant aroma, mainly through ethyl (E)-cinnamate, ethyl isovalerate, ethyl phenacetate with the higher odor activity values, while LFA promoted the yield by 13.2 % and resulted in a purer and less intense aroma through the aroma-active ß-damascenone, ethyl heptoate, ethyl phenacetate. These results facilitated the regulated mechanism of SFJ and LFA on Baijiu brewing and indicated that the used functional strains in this study could be applicated in SFJ way for the further industrial-scale application.

The active synergetic microbiota with Aspergillus as the core dominates the metabolic network of ester synthesis in medium-high temperature Daqu.

The active ester-synthesis microorganisms in medium-high temperature Daqu (MHT-Daqu) largely impact the strong-flavor Baijiu quality, while their actual composition and metabolic mechanism remain unclear. Here, to explore how the active microbiota contributes to MHT-Daqu ester biosynthesis, metatranscriptomic and metaproteomic analyses coupled with experimental verification were performed. The results showed that the MHT-Daqu microbiota with the higher ester-forming ability exhibited a more active dynamic alteration from transcription to translation. The genera Aspergillus, Bacillus, Leuconostoc, and Pediococcus could transcribe and translate obviously more ester-forming enzymes. In the ester-synthesis metabolic network, the synergetic microbiota confirmed by interaction analysis, containing Eurotiales, Bacillales, and Saccharomycetales, played an essential role, in which the Eurotiales and its representative genus Aspergillus contributed the highest transcript and protein abundance in almost every metabolic process, respectively. The recombined fermentation verified that their corresponding genera could produce the ester and precursor profiles very close to that of the original MHT-Daqu active microbiota, while the microbiota without Aspergillus caused a polar separation. These results indicated that the synergetic microbiota with Aspergillus as the core dominated the metabolic network of ester synthesis in MHT-Daqu. Our study provides a detailed framework of the association between the active synergetic microbiota and ester synthesis in MHT-Daqu.

Effects of six commercially available koji (Chinese Xiaoqu) on the production of ethyl acetate, ethyl lactate, and higher alcohols in Chinese Baijiu (distilled spirit) brewing.

Commercial koji has been increasingly used in Chinese Baijiu brewing; however, there are only few studies comparing different koji and their relationship with key components of Chinese Baijiu such as ethyl acetate, ethyl lactate, and higher alcohols. Here, we studied six commercially available koji and showed that the microbial communities in the individual koji varied in composition, with Rhizopus, Aspergillus, and Bacillus primarily associated with starch hydrolysis and Saccharomyces mainly associated with alcohol production. In the brewing processes using the six koji, Saccharomyces was undoubtedly the most abundant fungus and Weissella, Bacillus, and Acinetobacter were the predominant bacterial groups. The levels of ethyl acetate, ethyl lactate, and higher alcohols in all brewing processes using the koji exhibited rapid increase in the early stages of fermentation, which stabilized in the later stages, followed by substantial increase after distillation. The results of metagenomic and redundancy analyses of samples taken during the brewing processes indicated that Saccharomyces from the koji was closely related to the production of ethyl acetate, ethyl lactate, and higher alcohols. This study provides a basis for the quality improvement and application of commercial koji.

Contrasting the microbial community and non-volatile metabolites involved in ester synthesis between Qing-flavor Daqu and Nong-flavor Daqu.

Daqu, a fermentation starter, was important source of key flavors of Chinese Baijiu. The quality of Chinese Baijiu could be significantly affected by the ester-synthesis microorganisms. In order to clarify the microbial community that promoted the ester formation in Daqu, the dynamic changes of microbial community and non-volatile profiles of Qing-flavor Daqu and Nong-flavor Daqu samples through the whole making process were investigated by Illumina MiSeq platform and liquid chromatograph-mass spectrometry (LC-MS). The non-volatile compounds related to ester synthesis were identified by comparing with ester synthesis pathway and partial least squares discriminant analysis (PLS-DA). Correlations between microbial community and non-volatile metabolites involved in ester synthesis of two types of Daqu were disclosed by Pearson correlation analysis. Results showed that a total of 50 key compounds involved in ester synthesis were identified and 25 primary functional microorganisms were screened in 39 samples. Among them, in Qing-flavor Daqu, the top three primary functional microorganisms that had strong correlations with ester-formation precursors were Lactobacillus, Pantoea, and Sphingomonas; Lactobacillus and Pantoea had significantly positive interactions with various microorganisms, but Sphingomonas did not interact with others. In Nong-flavor Daqu, the top three primary functional microorganisms that had strong correlations with ester-formation precursors were Candida, Apiotrichum, and Cutaneotrichosporon. Candida showed strong positive correlation with other microorganisms, whereas Apiotrichum and Cutaneotrichosporon had no interaction with other microorganisms. The study could help our understanding of the microbial metabolism process in Daqu and provided a scientific basis for a controllable and feasible fermentation system.

Integrating metabolomics and metatranscriptomics to explore the formation pathway of aroma-active volatile phenolics and metabolic profile during industrial radish paocai fermentation.

The aroma profile of industrial Sichuan paocai is formed and regulated by complex physiological and biochemical reactions and microbial metabolism, but little is known so far. In this study, we comprehensively analyzed the changes of metabolic profile and gene expression profile, mainly explored the formation pathways of two skeleton aroma-active compounds, 4-ethylphenol and 4-ethylguaiacol, and verified the pathways at multiple levels. The results showed that a total of 136 volatile metabolites and 560 non-volatile metabolites were identified in the whole fermentation process. The types and concentrations of metabolites in paocai were higher than those in brine, and gradually converged with fermentation. Differential analysis of metabolism and transcription levels were both enriched in three pathways: amino acid metabolism, phenylpropanoid metabolism and lipid metabolism. Among them, 4-ethylphenol and 4-ethylguaiacol, the products of the phenylpropanoid metabolism, were converted from p-coumaric acid and ferulic acid in plant cell walls, respectively. Under the action of decarboxylase produced by yeast (such as Debaryomyces Hansenii) and lactic acid bacteria (such as Lactobacillus versmoldensis), intermediate metabolites vinylphenols were produced, and the intermediate metabolites further produce the final products under the action of vinylphenol reductase. The key gene copy number, enzyme activity, and metabolite concentration in the pathways were detected to provide stronger evidence for the formation pathways. This study provided meaningful new insights for the development of aroma-producing enzymes and further guidance for the flavor improvement of industrial paocai.

Microbial diversity in jiuqu and its fermentation features: saccharification, alcohol fermentation and flavors generation.

Chinese Baijiu, the national liquor of China, is also one of the world-renowned distilled spirits. Jiuqu, a fermentation starter, is the masterpiece of traditional food biotechnology with a long history in China. Compared to western brewing technology of using malt and yeast in stages, the mode of using jiuqu (or combined with pit mud, a activated sludge) for Baijiu brewing is recognized in China. So far, culture-dependent, molecular biology technology and omics approaches have provided deeper insights into study the jiuqu microbiome. Jiuqu is considered to be a microecosystem with diverse and unique microorganisms, in which fascinating features of saccharification, alcohol fermentation, and flavors generation appear. However, knowledge about microbial diversity of jiuqu and their roles involved in Baijiu fermentation is still fragmentary and not systematic enough. Therefore, this review introduced and compared three basic types of jiuqu starter: daqu, xiaoqu and fuqu. We described in detail the microbial succession during preparation of jiuqu, aiming to emphasize that succession process promotes to formation of its stable distribution of microbial community. We also summarized the main species originated from jiuqu and their various properties. Furthermore, reported results about fermentation features of saccharification, alcohol fermentation, and flavors generation in jiuqu microbiome were generalized, and these features were emphasized to play the potential role in Baijiu brewing. Although the current work is limited, promising clues can be traced for future investigation on comprehensive metabolic processes in jiuqu. KEY POINTS: • The various microorganisms present in jiuqu, and each has its specific property. • Microbial succession in preparation promotes to distribution of microbial community. • Jiuqu contributes the potential of saccharification, fermentation and flavors generation to Baijiu brewing.

Difference of microbial community and gene composition with saccharification function between Chinese nongxiangxing daqu and jiangxiangxing daqu.

BACKGROUND: The saccharification function of daqu is usually characterized by two indicators: saccharification power and liquefaction power. Daqu provides diverse microbial saccharifying enzymes for hydrolyzing carbohydrate in Baijiu fermenting grain. Obviously, the composition of microbial communities and enzymatic genes in different types of daqu cultured at varied temperatures is different. However, these differences in saccharification function are not fully understood. RESULTS: The findings suggested that the saccharification power and liquefaction power of jiangxiangxing daqu were lower than those of nongxiangxing daqu throughout the production process. We employed metagenomics to find evidence that a mode of multiple saccharifying enzymes involving amylase, cellulase and hemicellulase originating from various microbes exists in daqu. Moreover, a totality of 541 related differential genes were obtained, some of which, annotated to genera of Aspergillus, Lactobacillus and Weissella, were significantly enriched (P < 0.05) in nongxiangxing daqu, while others, annotated to thermophilic genera of Virgibacillus, Bacillus, Kroppenstedtia and Saccharopolyspora, showed a higher relative abundance in jiangxiangxing daqu (P < 0.05). CONCLUSION: Various microbial communities of daqu showed diverse saccharification capacity during cultivation of different parameters. These findings are helpful in comprehending the saccharification functional genes of daqu. © 2022 Society of Chemical Industry.

Temperature-dependent alcohol acyltransferase reactions as the main enzymatic way to produce short-chain (C4-C8) and medium-chain (C9-C13) esters over the whole Daqu-making process.

BACKGROUND: The ester-synthesis enzymes influenced by environmental factors during Daqu-making process largely determine the flavor of Chinese liquor, but the main ester-synthesis enzyme and its key influencer remain unclear. Here, the volatile ester profiles over the whole Daqu-making process, under different treatments, for at least 90 days, were carefully analyzed, and the potential ester-synthesis enzymes, as well as their dependently environmental factors, were explored. RESULTS: In the detected 46 volatile esters, only the short-chain (C4-C8) and medium-chain (C9-C13) ester content obviously changed, as the primary contributor discriminating different samples. Their trends were both consistent with that of the alcohols and the primary metabolism, which included alcohol acyltransferases (AATs) reaction with alcohols and acyl-CoAs as the substrates. Among the potential ester-synthesis enzymes, the typical AAT activity also exhibited the highest correlation with the short- and medium-chain esters (r > 0.78, P < 0.05). The Mantel test between environmental factors and ester production showed that temperature of Daqu was directly correlated with the short-chain esters (r = 0.58, P < 0.01) and AAT activity (r = 0.56, P < 0.01). Further, the short- and medium-chain ester content in Daqu under the treatment nearer to the reported optimal temperature of 40-50 °C of AATs reaction was overall higher than that of the other treatment Daqu. CONCLUSION: This study revealed that the temperature-dependent AATs reaction was the main enzymatic method producing the short- and medium-chain esters over the whole Daqu-making process. The results could contribute to the flavor improvement of Baijiu. © 2022 Society of Chemical Industry.

Bioinformatics analysis of amino acid decarboxylases related to four major biogenic amines in pickles.

Microbial amino acid decarboxylases (AADs) produce biogenic amines (BAs) in fermented food. However, a systematic comparison of the AADs' properties from different microorganisms in pickle fermentation remains unexplored. Here, we bioinformatically analyzed the amino acid sequences of AADs corresponding to four major BAs for common microorganisms in pickle fermentation. We showed that their sequences, besides tyrosine decarboxylase, differed among microorganisms. Overall, the AAD sequences varied lesser among bacterial species than between bacteria and fungi, with those in Lactobacillus sharing occasionally high similarity with other bacteria. Most AADs were predicted as stable cytosolic endoenzymes. Molecular docking showed that most commonly used spice components in pickle production, especially pepper, chili, and ginger, strongly bind to the AAD active sites, thus may inhibit the enzymes and reduce the BA accumulation. This study provides insights for deeply understanding the different microbial AAD properties in pickle fermentation and reducing BAs by appropriately using spices.

Analysis of fermentation control factors on volatile compounds of primary microorganisms in Jiang-flavor Daqu.

Chinese Jiang-flavor Baijiu is the most widely consumed liquor. Jiang-flavor Daqu, a fermentation starter, is important sources of key flavors of Jiang-flavor Baijiu. Some microbes play significant roles in flavor formation of Daqu. In order to clarify the microbial population that promotes the formation of Daqu flavor, we use high throughput sequencing technology combined with headspace solid-phase microextraction gas chromatography-mass spectrometry to investigate microbial population and volatile compounds in Jiang-flavor Daqu. In addition, the dynamic changes of physicochemical factors and enzyme activities in Jiang-flavor Daqu were investigated. Correlations between microbial population, volatile compounds, physicochemical factors, and enzyme activities of Jiang-flavor Daqu were disclosed by redundancy analysis and Spearman correlation analysis. A total of 66 volatile compounds were identified and 14 primary microorganisms were selected. Results showed that high temperature environment could promote the formation of acids, aldehydes and ketones, phenols, furans by affecting the growth of Monascus, Trichomonascus, Cutaneotrichosporon, Wallemia, Millerozyma, Nigrospora, Cladosporium, Bacillus, and Pediococcus in the early fermentation stage. While high nitrogen environment was more suitable for the growth of Virgibacillus and Kroppenstedtia, who could promote the formation of pyrazines in the late fermentation stage. PRACTICAL APPLICATIONS: This study has provided a scientific basis for the directed regulation of Daqu fermentation through physicochemical factors, developed scientific basis for artificially constructing Daqu microbial population and obtaining an easy-to-operate, reproducible fermentation system for Daqu production.

Study on the Effect of Key Genes ME2 and adhE during Luzhou-Flavor Baijiu Brewing.

Luzhou-flavor baijiu (LFB) is brewed by the combined action of various microorganisms, and its flavor is affected by the microbial community and the genes they express, but which genes are the key ones during LFB brewing is less clear. Based on our previous studies the genes ME2 and adhE were identified as key genes, but which role they play was also unknown. In this study functional microorganisms were screened based on the key genes ME2 and adhE, and they were identified to be Rummeliibacillus suwonensis, Clostridium tyrobutyricum and Lactobacillus buchneri. Then simulated fermentation experiments were carried out with the functional microorganisms, and during the fermentation process expression of the key genes and the amounts of the main flavors were detected to analyze the role of the key genes. The results showed that the key gene ME2 was significantly positively correlated with the contents of the main acids, however the key gene adhE and the formation of the main esters in the LFB brewing process was a significant positive correlation. This study verified the two key genes ME2 and adhE complement each other in the LFB brewing process, playing an important role in promoting the formation of flavor substances, and are very beneficial to improve the quality of LFB.

Characterization of aroma and bacteria profiles of Sichuan industrial paocai by HS-SPME-GC-O-MS and 16S rRNA amplicon sequencing.

Sichuan industrial paocai and traditional home-made paocai have different aroma profiles due to different manufacturing techniques, but detailed information about the aroma profiles and aroma-producing microorganism of Sichuan industrial paocai remain largely elusive. For this reason, we established and validated an external standard method of headspace solid-phase microextraction gas chromatography-mass spectrometry (HS-SPME-GC-MS) combined with gas chromatography-olfactometry (GC-O) for identification and accurate quantitation of aroma-active compounds in Sichuan industrial paocai. This method was combined with 16S rRNA amplicon sequencing to comprehensively analyze the aroma and bacteria profiles of Sichuan industrial paocai. A total of 121 volatile compounds were identified, among which 36 odorants were identified as aroma-active compounds with aroma intensities (AIs) ranging from 0.67 to 5.00 by GC-O. The types of aroma-active compounds in Sichuan industrial paocai were variety-specific to some extent, but the aroma-active compounds shared by different varieties of Sichuan industrial paocai (i.e., skeleton aroma-active compounds) were phenylethyl alcohol, acetic acid, butanoic acid, 2-methylbutanoic acid, ethyl hexanoate, 4-ethylphenol and 4-ethylguaiacol. Moreover, 17 key aroma-active compounds of AI > 1 in radish paocai were quantitated by external standard method, and their odor activity values (OAVs) were calculated based on the odor thresholds. Further, 12 aroma-active compounds with OAV ≥ 1 in one of the radish paocai were selected to construct the recombination model, which revealed good agreement with the original sample. Furthermore, Lactobacillus, Pediococcus, Pseudomonas and Sphingomonas were the dominant bacteria in Sichuan industrial paocai. Correlation analysis between 16 dominant bacteria and 36 aroma-active compounds showed that Pediococcus, Arcobacter and Lactobacillus could be the core aroma-producing bacteria of Sichuan industrial paocai.

Analysis of the difference between aged and degenerated pit mud microbiome in fermentation cellars for Chinese Luzhou-flavor baijiu by metatranscriptomics.

BACKGROUD: Chinese Luzhou-flavor baijiu (LFB) was fermented in an underground cellar, and the bottom and side of the cellar were covered with pit muds (PMs), where the metabolic activity of the microorganisms had a significant effect on the LFB quality. PMs can be divided into aged pit mud (AP) and degenerated pit mud (DP), thus, the qualities of LFB generated from AP and DP were different. In this essay, metatranscriptomics method was applied to illustrate the differences of the two PMs, as well as to search out the pivotal microorganisms and genes influencing the quality of LFB. RESULTS: Archaea, Clostridium and some thermophilic microorganisms might bring significant effect in AP, while the active eukaryota and Anaeromyxobacter would cause degeneration in PM. Also, the metabolism of carbohydrate and amino acid were more active in AP. What is more, carbohydrate, amino acid and their derivant can produce important organic acids via the activity of the microorganisms in PMs. There were eight critical enzymes noticed in the organic acids metabolic pathway, which were more actively expressed in AP, demonstrating active expression of the critical genes related to organic acid metabolism could have a positive effect on LFB quality. CONCLUSION: This study identified specific differences in active microorganisms, active expressed genes and the expression levels of key genes in vital metabolic pathway between AP and DP. Which may be the actual reason for the differences in the quality of LFB made from different PMs. Mastering these results will provide assistance to improve the quality of LFB. © 2021 Society of Chemical Industry.

Effect of Pit Mud on Bacterial Community and Aroma Components in Yellow Water and Their Changes during the Fermentation of Chinese Strong-Flavor Liquor.

As the main by-product of Chinese strong-flavor liquor, yellow water plays an important role in the formation of flavor components. Yellow water from different fermentation periods (30th day, 45th day, 60th day) was selected to analyze the aroma components by Headspace solid phase micro-extraction Gas Chromatography-Mass Spectrometry, and the microorganism community was evaluated by high-throughput sequencing technology and bioinformatics analysis of DNA. As the fermentation time was prolonged, the main flavor components significantly increased, and the amount of the common microbial population between yellow water and pit mud increased gradually. Among the common microorganisms, Lactobacillus accounted for the largest proportion, at about 56.96%. The microbes in the yellow water mainly belonged to Firmicutes. The abundance of Bacilli (the main bacteria) gradually decreased with time, at 87.60% at the 30th day down to 68.87% at the 60th day, but Clostridia gradually increased from 10.29% to 27.48%. At the genus level, some microbes increased significantly from the 30th day to 60th day, such as Caproiciproducens, which increased from 2.65% to 6.30%, and Sedimentibacter, increasing from 0.47% to 2.49%. RDA analysis indicated that the main aroma components were positively correlated with Clostridia and negatively correlated with Bacilli.

Gradient heterostructure perovskite single crystals enable the improvement of radiative recombination for scintillator application.

Recently, organic-inorganic hybrid perovskites (OIHPs) are rising as promising candidates for light-emitting applications, due to their superior optical properties. High performance light-emitting applications such as scintillators require minimum non-radiative recombination and high fractions of radiative recombination. Here, we report a simple solution-processing strategy for the synthesis of funnel-type CH3NH3(MA)PbCl3/CH3NH3(MA)PbBrxCl3-x heterostructure perovskite materials that improve the light emission performances. The single crystal X-ray diffraction pattern indicates that the lattice mismatch is only ∼3.24% in the heterointerface. The halide gradient is helpful for driving the photoexcited carriers from the internal high bandgap material to the low bandgap light-emitter layer. The steady-state photoluminescence (PL) and radioluminescence (RL) spectra show that the luminescence intensity has been significantly improved by this heterostructure perovskite. Time-resolved photoluminescence (TRPL) exhibits carrier transport along the halide gradient. Our research suggests that the gradient halide perovskite heterostructure with specific optical properties could be a prospect for commercial scintillator applications.

Bulk Organic-Inorganic Methylammonium Lead Halide Perovskite Single Crystals for Indirect Gamma Ray Detection.

Scintillators that convert ionization radiation photons to UV-visible photons have attracted extraordinary attention. Traditional scintillators are associated with a vacuum photomultiplier tube that faces strict constraints of fragility, magnetic fields, and operated voltage, or coupled to a silicon photomultiplier (SiPM) with optical silicone grease. Here, we report a high-performance radiation detector with an indirect photon-to-photon conversion radiation detection model based on perovskite single crystals (SCs), where perovskite SCs have been directly integrated into the window of SiPM by using the solution growth method at low temperature. Tunable X (γ)-ray excited light emission in the range of 414 to 600 nm is obtained with different concentrations of Br doping, which greatly matches the response wavelength of SiPM. Small Br-doped CH3NH3PbBr0.05Cl2.95 SCs exhibit high transmittance and weak self-absorption, resulting in improved scintillation light emissions. Moreover, we have successfully collected a 137Cs source gamma-ray pulse height spectrum with the SiPM readout. The MAPbBr0.05Cl2.95 scintillator exhibits a decay time of 0.14 ± 0.02 ns and a light yield of 18 000 photons/MeV with an energy resolution of 10.5 ± 0.4% at 662 keV. The results indicate that the CH3NH3PbBrxCl3-x perovskite SCs could enable the next generation of low-cost, fast, and fine-energy resolution scintillators.

High-Performance Surface Barrier X-ray Detector Based on Methylammonium Lead Tribromide Single Crystals.

Hybrid methylammonium lead tribromide (MAPbBr3) perovskite has attracted great attention in ionization radiation detection. However, the charge collection remains a challenge. Here, fast response and high-sensitivity X-ray detection based on MAPbBr3 single crystals with a surface barrier Schottky diode has been achieved at room temperature. The Schottky surface barrier can overcome the large leakage current at a high electrical field, enabling us to reduce the noise and increase the charge collection efficiency. This surface barrier device has been demonstrated a 3 times improvement over the photoconductor based X-ray detector, which enables usage in nuclear medicine, especially for X-ray imaging technology.

Raman Spectroscopy of Multi-Layer Graphene epitaxially Grown on 4H-SiC by Joule Heat Decomposition.

We developed a Joule heating decomposition (JHD) method, which applied direct current on the SiC for the epitaxial growth of multi-layer graphene (MLG) films on Si-terminated (0001) face of the high doping 4H-SiC substrate. By this JHD method, the growth time for preparing MLG was only several minutes. Raman spectroscopy was employed to study the influence of the temperature caused by the Joule heating on the quality and the uniformity of the sample. Then, other properties, such as the strain, the layer's number, and the electric characteristics, of the MLG were studied in details. It was found that the quality of the MLG was substantially dependent on the growth temperature (operation current) and the growth time, while the layer's number was only dependent on the growth temperature but not the growth time. Finally, less-defect and homogeneous MLG (~ 45 layers) with an area of ~ 12 × 5 mm2 could be obtained at a heating temperature of ~ 1470 °C with duration time of 5 min. By using the linear transmission line method, the specific contact resistance of Au and MLG was 5.03 × 10-5 Ω cm2, and the sheet resistance was 52.36 Ω/sq, respectively.