ABSTRACT
In this work, we focus on the understanding of the driving force behind the S1-T1 excited-state energy inversion (which would thus violate Hund's rule, making the S1 state lower in energy than the T1 state) of two non-benzenoid non-alternant hydrocarbons, composed of odd-membered rings. The molecules considered here have identical chemical composition but different atomic configuration in space. The delicate interplay between structural and electronic factors that might induce inversion and its energy extension, only by a few meV, is systematically investigated here by state-of-the-art calculations. Qualitative and quantitative accurate predictions are obtained employing post-HF methods, thanks to the balanced and careful inclusion of electron correlation effects. The obtained results might guide and rationalize new searches for molecules violating Hund's rule, concomitantly demonstrating the importance of key contributions from the theoretical method of choice.
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Cardiotocography , Heart Rate, Fetal , Pregnancy , Female , Humans , Cardiotocography/methods , Gestational AgeABSTRACT
This study comprises a critical review of modeling of pesticides in surface waters. The aim was to update the status of the use of models to simulate the fate of pesticides from diffuse sources. ISI papers were selected on Scopus and the information concerning the study areas, type of pesticides (herbicides, fungicides and insecticides), the model, and the methodology adopted (i.e., calibration and/or validation, spatial and temporal scales) were analyzed. The studies were carried out in Europe (55.5%), North America (22.3%), Asia (13.9%) and South America (8.3%). The Soil and Water Assessment Tool proved to be the most used model (45.95%). Herbicides were the most modeled pesticides (71.4%), followed by insecticides (18.2%) and fungicides (10.4%). The main herbicides modeled were atrazine, metolachlor, isoproturon, glyphosate, and acetochlor. Insecticides such as chlorpyrifos and metaldehyde. Chlorothalonil, and fungicides (i.e., tebuconazole) were the most widely investigated. Based on published studies, it was found that modeling approaches for assessing the fate of pesticides are constantly evolving and the model algorithms work well with diverse watershed conditions, management strategies, and pesticide properties. Several papers reported concentrations of pesticides exceeding ecotoxicological thresholds revealing that water contamination with pesticides used in agriculture and urban areas is a priority issue of current global concern.
Subject(s)
Fungicides, Industrial , Herbicides , Insecticides , Pesticides , Water Pollutants, Chemical , Pesticides/analysis , Fungicides, Industrial/analysis , Insecticides/analysis , Environmental Monitoring/methods , Fresh Water , Herbicides/analysis , Agriculture , Water , Water Pollutants, Chemical/analysisABSTRACT
OBJECTIVES: To assess natural history and 12-month change of a series of scales and functional outcome measures in a cohort of 117 patients with primary mitochondrial myopathy (PMM). METHODS: Twelve months follow-up data of 117 patients with PMM were collected. We analysed the 6-min walk test (6MWT), timed up-and-go test (× 3) (3TUG), five-times sit-to-stand test (5XSST), timed water swallow test (TWST), and test of masticating and swallowing solids (TOMASS) as functional outcome measures; the Fatigue Severity Scale and West Haven-Yale Multidimensional pain inventory as patient-reported outcome measures. PMM patients were divided into three phenotypic categories: mitochondrial myopathy (MiMy) without extraocular muscles involvement, pure chronic progressive external ophthalmoplegia (PEO) and PEO&MiMy. As 6MWT is recognized to have significant test-retest variability, we calculated MCID (minimal clinically important difference) as one third of baseline 6 min walking distance (6MWD) standard deviation. RESULTS: At 12-month follow-up, 3TUG, 5XSST and FSS were stable, while TWST and the perceived pain severity (WHYMPI) worsened. 6MWD significantly increased in the entire cohort, especially in the higher percentiles and in PEO patients, while was substantially stable in the lower percentile (< 408 m) and MiMy patients. This increase in 6MWD was considered not significant, as inferior to MCID (33.3 m). NMDAS total score showed a slight but significant decline at 12 months (0.9 point). The perceived pain severity significantly worsened. Patients with PEO performed better in functional measures than patients with PEO&MiMy or MiMy, and had lower values of NMDAS. CONCLUSIONS: PMM patients showed a slow global decline valued by NMDAS at 12 months; 6MWT was a more reliable measurement below 408 m, substantially stable at 12 months. PEO patients had better motor performance and lower NMDAS than PEO&MiMy and MiMy also at 12 months of follow-up.
Subject(s)
Mitochondrial Myopathies , Ophthalmoplegia, Chronic Progressive External , Humans , Follow-Up Studies , Walk Test/methods , Mitochondrial Myopathies/complications , Mitochondrial Myopathies/diagnosis , Time Factors , WalkingSubject(s)
Suicide, Assisted , Embryo, Mammalian , Humans , Italy , Reproductive Techniques, AssistedABSTRACT
The energy difference (ΔEST) between the lowest singlet (S1) state and the triplet (T1) excited state of a set of azaphenalene compounds, which is theoretically and experimentally known to violate Hund's rule, giving rise to the inversion of the order of those states, is calculated here with a family of double-hybrid density functionals. That excited-state inversion is known to be very challenging to reproduce for time-dependent density functional theory employing common functionals, e.g., hybrid or range-separated expressions, but not for wavefunction methods due to the inclusion of higher-than-single excitations. Therefore, we explore here if the last developed family of density functional expressions (i.e., double-hybrid models) is able to provide not only the right excited-state energy order but also accurate ΔEST values, thanks to the approximate inclusion of double excitations within these models. We herein employ standard double-hybrid (B2-PLYP, PBE-QIDH, and PBE0-2), range-separated (ωB2-PLYP and RSX-QIDH), spin-scaled (SCS/SOS-B2PLYP21, SCS-PBE-QIDH, and SOS-PBE-QIDH), and range-separated spin-scaled (SCS/SOS-ωB2-PLYP, SCS-RSX-QIDH, and SOS-RSX-QIDH) expressions to systematically assess the influence of the ingredients entering into the formulation while concomitantly providing insights for their accuracy.
ABSTRACT
OBJECTIVE: Understanding the evolutionary dynamics of the Coronavirus disease 2019 (COVID-19) pandemic in the coming months is a matter of great importance and urgency for governments worldwide, making fundamental decisions based on what is known about the transmission mechanisms of the virus and its survival in the environment. The present study aimed to evaluate the impact of demographic variables, solar radiation and relative humidity on the spread of the COVID-19 pandemic of the various regions in Italy. MATERIALS AND METHODS: The retrospective longitudinal study was conducted, and data used in this study was obtained from the Italian Health Ministry. Descriptive statistics included mean, frequency, and percentage, and results presented by graphs were calculated. RESULTS: The infection trend was investigated by comparing it with the demographic situation and the irradiation indices of solar ultraviolet light that are detected with the changing seasons. The present study reported that the geographic areas with higher population density and lower solar radiation during the autumn and winter months were most affected by SARS-CoV-2. CONCLUSIONS: The analysis carried out can provide a predictive model for the future phases of the COVID-19 pandemic in Italy, regardless of the adoption of lockdown measures and behavioral factors.
Subject(s)
COVID-19/transmission , Disease Outbreaks/prevention & control , Meteorological Concepts , Seasons , COVID-19/diagnosis , COVID-19/epidemiology , COVID-19/virology , Disease Outbreaks/statistics & numerical data , Humans , Italy/epidemiology , Longitudinal Studies , Population Density , Predictive Value of Tests , Quarantine/statistics & numerical data , Retrospective Studies , SARS-CoV-2/genetics , Ultraviolet Rays/adverse effectsABSTRACT
The energy difference between singlet and triplet excitons, or ΔEST, is a key parameter for novel light-emission mechanisms (i.e., TADF or thermally activated delayed fluorescence) or other photoactivated processes. We have studied a set of conjugated molecules (peri-acenoacenes and their heteroatom-doped analogues) to observe the evolution of their excited-state properties upon increasing the system size with and without substitution with a pair of N atoms. Since these molecules exhibit a (ground-state) diradicaloid character, together with marked correlation effects influencing the excited-states formed, we have applied a variety of theoretical methods (FT-DFT, TD-DFT, SF-TD-DFT, CIS, CIS(D), SCS-CC2, SA-CASSCF, and SC-NEVPT2) to bracket the accuracy of the results while concomitantly providing insights into electronic structure. The results show how this chemical strategy (N-doping) largely modifies not only the excited-state energies but also the oscillator strengths and the ΔEST values, constituting versatile platforms for fine-tuned photophysical applications.
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OBJECTIVE: New fentanyl analogues have been constantly emerging into the illegal drug market as cheap substitutes of heroin posing a serious health threat for consumers because of their high toxicity. Analytical methods to disclose the presence of these compounds in biological fluids of intoxicated individuals need to be updated to keep up with the new trends. In this study, we updated an ultra-high-performance liquid chromatography-tandem mass spectrometry method previously developed, for detecting some new fentanyl analogues and metabolites (sufentanil and norsufentanil, cis-3-methylnorfentanyl, trans-3-methylnorfentanyl, metabolites of cis and transmethylfentanyl, beta-phenylfentanyl, phenylfentanyl, para-fluoro furanyl fentanyl, isobutyryl fentanyl and ocfentanil) in urine sample. MATERIALS AND METHODS: Urine samples were simply diluted before injection in the chromatograph equipped with a reversed phase microcolumn. Detection was achieved with a triple quadrupole mass spectrometer with an electrospray ionization source in positive ion mode and operated in multiple reaction monitoring. RESULTS: The chromatographic separation was short (5 min) and the method was fully validated with a high sensitivity being limits of quantifications from 0.003 to 0.006 µg/L urine for the analytes under investigation. CONCLUSIONS: The suitability of the method was tested with urine specimens from former heroin addicts, which resulted positive by immunological screening to the class of fentanyl analogues. This method represents a valid tool to document recent exposure to the above-reported compounds for clinical and forensic purposes.
Subject(s)
Fentanyl/urine , Calibration , Chromatography, High Pressure Liquid , Fentanyl/metabolism , Humans , Quality Control , Tandem Mass SpectrometryABSTRACT
OBJECTIVE: The inhibition of the metastatic capability of cancer cells is a pivotal aim of current anticancer strategies. We investigated herein the anti-migrating and anti-invasive properties of Zebrafish embryo extracts (SL) - an integrative formula comprising morphogenetic factors extracted from zebrafish embryos - alone or in association with 5-Fluoro-Uracil (5-FU), when added to metastatic breast cancer cells (MDA-MB-231) and in normal epithelial breast cells (MCF10A) committed toward an inflammatory phenotype upon TGF-ß1 stimulation. MATERIALS AND METHODS: Invasiveness, migrating capability, cytoskeleton architecture and related molecular factors involved in the epithelial-mesenchymal transition were studied after treatment with 5-FU, with and without SL. RESULTS: Remarkably, in both circumstances, embryo extracts amplify the migratory inhibition triggered by the anticancer drug 5-Fu. The fact that such an effect is noticed in normal as well as in cancerous cells suggests that the critical target of embryo extracts is specifically represented by the migrating/invasive phenotype. However, while 5-FU was unable in antagonizing the invasiveness of cancerous cells, the association with SL can significantly impair the invasive capability of tumor cells. These findings are noticeably associated with the reversion of the EMT phenotype in SL-treated cells, as documented by the contemporary downregulation of TCTP and some EMT-related molecular effectors, like α-SMA and Vimentin. CONCLUSIONS: Embryo fish extracts significantly counteract the migrating and invasive phenotype of cancerous and inflammatory breast cells treated with the chemotherapeutic drug 5-FU. The availability of a compound able to amplify 5-Fu activity while significantly hampering the invasive phenotype of breast cancer should provide invaluable benefits, namely if we consider that this compound is substantially deprived of side-effects.
Subject(s)
Antimetabolites, Antineoplastic/pharmacology , Breast Neoplasms/drug therapy , Fluorouracil/pharmacology , Animals , Breast Neoplasms/pathology , Cell Line , Cell Movement/drug effects , Cell Proliferation/drug effects , Cell Survival/drug effects , Drug Screening Assays, Antitumor , Female , Humans , Zebrafish/embryologySubject(s)
COVID-19 , Health Services Accessibility/organization & administration , Remote Consultation/organization & administration , SARS-CoV-2 , Telemedicine/organization & administration , COVID-19/prevention & control , COVID-19/transmission , Health Services Accessibility/standards , Humans , Physician-Patient Relations , Remote Consultation/standards , Telemedicine/standardsABSTRACT
The full harvesting of both singlet and triplet excitons can pave the way toward more efficient molecular light-emission mechanisms (i.e., TADF or thermally activated delayed fluorescence) beyond the spin statistics limit. This TADF mechanism benefits from low (but typically positive) singlet-triplet energy gaps or ΔEST. Recent research has suggested the possibility of inverting the order of the energy of lowest singlet and triplet excited states, thus opening new pathways to promote light emission without any energy barrier through triplet to singlet conversion, which is systematically investigated here by means of theoretical methods. To this end, we have selected a set of heteroatom-substituted triangle-shaped molecules (or triangulenes) for which ΔEST < 0 is predicted. We successfully rationalize the origin of that energy inversion and the reasons for which theoretical methods might produce qualitatively inconsistent predictions depending on how they treat n-tuple excitations (e.g., the large contribution of double excitations for all of the ground and excited states involved). Unfortunately, the time-dependent density functional theory method is unable to deal with the physical effects driving this behavior, which prompted us to use more sophisticated ab initio methods here such as SA-CASSCF, SC-NEVPT2, SCS-CC2, and SCS-ADC(2).
ABSTRACT
PURPOSE: SARS-COV-2 is a pathogenic agent belonging to the coronavirus family, responsible for the current global world pandemic. Angiotensin-converting enzyme 2 (ACE-2) is the receptor for cellular entry of SARS-CoV-2. ACE-2 is a type I transmembrane metallo-carboxypeptidase involved in the Renin-Angiotensin pathway. By analyzing two independent databases, ACE-2 was identified in several human tissues including the thyroid. Although some cases of COVID-19-related subacute thyroiditis were recently described, direct proof for the expression of the ACE-2 mRNA in thyroid cells is still lacking. Aim of the present study was to investigate by RT-PCR whether the mRNA encoding for ACE-2 is present in human thyroid cells. METHODS: RT-PCR was performed on in vitro ex vivo study on thyroid tissue samples (15 patients undergoing thyroidectomy for benign thyroid nodules) and primary thyroid cell cultures. RESULTS: The ACE-2 mRNA was detected in all surgical thyroid tissue samples (n = 15). Compared with two reporter genes (GAPDH: 0.052 ± 0.0026 Cycles-1; ß-actin: 0.044 ± 0.0025 Cycles-1; ACE-2: 0.035 ± 0.0024 Cycles-1), the mean level of transcript expression for ACE-2 mRNA was abundant. The expression of ACE-2 mRNA in follicular cells was confirmed by analyzing primary cultures of thyroid cells, which expressed the ACE-2 mRNA at levels similar to tissues. CONCLUSIONS: The results of the present study demonstrate that the mRNA encoding for the ACE-2 receptor is expressed in thyroid follicular cells, making them a potential target for SARS-COV-2 entry. Future clinical studies in patients with COVID-19 will be required for increase our understanding of the thyroid repercussions of SARS-CoV-2 infection.
Subject(s)
Angiotensin-Converting Enzyme 2/analysis , COVID-19/complications , RNA, Messenger/analysis , Receptors, Virus/analysis , Thyroiditis, Subacute/etiology , Adult , COVID-19/metabolism , Female , Humans , Male , Primary Cell Culture , Real-Time Polymerase Chain Reaction , Thyroid Gland/chemistry , Thyroid Gland/cytology , Thyroidectomy , Thyroiditis, Subacute/metabolismABSTRACT
PURPOSE: Per- and poly-fluoroalkyl-substances (PFASs) are synthetic compounds that raised concern due to their potential adverse effects on human health. Long-chain PFAS were banned by government rules in many states, and thus, new emerging PFAS were recently introduced as substitutes. Among these, Perfluoro{acetic acid, 2-[(5-methoxy-1,3-dioxolan-4-yl)oxy]}, ammonium salt (C6O4) was recently introduced to produce a range of food contact articles and literature data about this compound are scanty. The aim of this study was to evaluate the in vitro effects of exposure to C6O4, compared with PFOA and PFOS on thyroid cells. METHODS: FRTL5 rat-thyroid cell lines and normal human thyroid cells (NHT) were incubated with increasing concentrations of C6O4 for 24, 48, 72, and 144 h to assess cell viability by WST-1. Cell viability was confirmed by AnnexinV/PI staining. Long-chain PFAS (PFOA and PFOS) were used at same concentrations as positive controls. The proliferation of cells exposed to C6O4, PFOA, and PFOS was measured by staining with crystal violet and evaluation of optical density after incubation with SDS. Changes in ROS production by FRTL5 and NHT after exposure to C6O4 at short (10, 20, and 30 min) and long-time points (24 h) were evaluated by cytofluorimetry. RESULTS: C6O4 exposure did not modify FRTL5 and NHT cell viability at any concentration and/or time points with no induction of necrosis/apoptosis. At difference, PFOS exposure reduced cell viability of FRTL5 while and NHT, while PFOA only in FRTL5. FRTL5 and NHT cell proliferation was reduced by incubation with by PFOA and PFOS, but not with C6O4. ROS production by NHT and FRTL5 cells was not modified after C6O4 exposure, at any time/concentration tested. CONCLUSIONS: The present in vitro study constitutes the first evaluation of the potential adverse effects of the new emerging PFAS C6O4 in cultured rat and human thyroid cells, suggesting its safety for thyroid cells in vitro.
Subject(s)
Alkanesulfonic Acids , Caprylates , Cell Proliferation/drug effects , Fluorocarbons , Reactive Oxygen Species/analysis , Thyroid Gland , Alkanesulfonic Acids/chemistry , Alkanesulfonic Acids/toxicity , Animals , Caprylates/chemistry , Caprylates/toxicity , Cell Line , Cell Survival/drug effects , Endocrine Disruptors/analysis , Endocrine Disruptors/isolation & purification , Fluorocarbons/chemistry , Fluorocarbons/toxicity , Humans , Oxidative Stress/drug effects , Rats , Thyroid Gland/drug effects , Thyroid Gland/metabolismABSTRACT
We have investigated the origin of the S1 -T1 energy levels inversion for heptazine, and other N-doped π-conjugated hydrocarbons, leading thus to an unusually negative singlet-triplet energy gap ( ΔEST<0 ). Since this inversion might rely on substantial doubly-excited configurations to the S1 and/or T1 wavefunctions, we have systematically applied multi-configurational SA-CASSCF and SC-NEVPT2 methods, SCS-corrected CC2 and ADC(2) approaches, and linear-response TD-DFT, to analyze if the latter method could also face this challenging issue. We have also extended the study to B-doped π-conjugated systems, to see the effect of chemical composition on the results. For all the systems studied, an intricate interplay between the singlet-triplet exchange interaction, the influence of doubly-excited configurations, and the impact of dynamic correlation effects, serves to explain the ΔEST<0 values found for most of the compounds, which is not predicted by TD-DFT.
ABSTRACT
COVID-19 pandemic has underlined that unknown viral infections, which jump from animals to humans, can be extremely dangerous. In case of new viruses as SARS-CoV2, available drugs can fail to contrast the virus aggressiveness leading patients to death. Long time is necessary to create a vaccine, but immediate solutions are necessary to stop the mortality COVID-19 related. We have learned that the immune-system is the key to reduce the severity of COVID-19 and, through its modulation, it has been possible saving people's life. In this short communication, we discuss the use of nutraceuticals to modulate and stimulate the immune answer for reducing the severity of COVID-19 symptoms. The nutraceuticals are safe and can be administered to all ages. In addition, combination of natural anti-viral elements and immune-stimulating molecules already successfully tested against others upper-respiratory tract infections-could be efficient against SARS-CoV2. We believe that these natural molecules could really be a valid ally against COVID-19, especially in this moment in which a SARS-CoV2 vaccine is still not available.
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Coronavirus Infections/therapy , Dietary Supplements , Pneumonia, Viral/therapy , Antiviral Agents/chemistry , Antiviral Agents/pharmacology , Antiviral Agents/therapeutic use , Betacoronavirus/isolation & purification , COVID-19 , Coronavirus Infections/pathology , Coronavirus Infections/virology , Humans , Lactobacillus/physiology , Pandemics , Pneumonia, Viral/pathology , Pneumonia, Viral/virology , SARS-CoV-2 , Selenium/pharmacology , Selenium/therapeutic use , Severity of Illness Index , T-Lymphocytes/cytology , T-Lymphocytes/immunology , T-Lymphocytes/metabolism , Virus Replication/drug effectsSubject(s)
Betacoronavirus/pathogenicity , Coronavirus Infections/pathology , Estrogens/metabolism , Pneumonia, Viral/pathology , Betacoronavirus/isolation & purification , COVID-19 , Coronavirus Infections/virology , Epidermal Growth Factor/metabolism , Estrogens/pharmacology , Female , Humans , Lung/metabolism , Male , Nasal Mucosa/immunology , Nasal Mucosa/metabolism , Pandemics , Pneumonia, Viral/virology , Progesterone/pharmacology , Risk , SARS-CoV-2 , Virulence/drug effectsSubject(s)
Coronavirus Infections/mortality , Pneumonia, Viral/mortality , Sex Distribution , Betacoronavirus , COVID-19 , Comorbidity , Female , Humans , Italy/epidemiology , Male , Pandemics , SARS-CoV-2ABSTRACT
BACKGROUND: Gestational diabetes mellitus (GDM) is a common pregnancy complication characterized by hyperglycaemia with onset or first recognition during pregnancy. Risk factors include family history of diabetes, previous GDM, genetic predisposition for GDM/type 2 diabetes, insulin resistance conditions such as overweight, obesity and ethnicity. Women with GDM are at high risk for fetal macrosomia, small for gestational age, neonatal hypoglycaemia, operative delivery and caesarean delivery. The aim of this narrative review is to summarize the most recent findings of diagnosis and treatment of GDM in order to underline the importance to promote adequate prevention of this disease, especially through lifestyle interventions such as diet and physical activity. METHODS: The research was conducted using the following electronic databases, MEDLINE, EMBASE, Web of Science, Scopus, ClinicalTrial.gov, OVID and Cochrane Library, including all published randomized and non-randomized studies as well as narrative and systematic reviews. RESULTS: The lack of universally accepted criteria makes the definition of diagnosis and prognosis of this condition difficult. Early diagnosis and glucose blood level control may improve maternal and fetal short and long-term outcomes. Treatment strategies include nutritional interventions and exercise. Medical treatment can be necessary if these strategies are not effective. Moreover, novel non-pharmacologic agents such as myo-inositol seem to be effective and safe both in the prevention and the treatment of GDM. CONCLUSIONS: It is important to promote adequate prevention of GDM. Further studies are needed in order to better define the most appropriate strategies for the clinical management of women affected by GDM.
Subject(s)
Diabetes, Gestational , Early Medical Intervention/methods , Prenatal Care/methods , Preventive Health Services/methods , Diabetes, Gestational/diagnosis , Diabetes, Gestational/epidemiology , Diabetes, Gestational/prevention & control , Diabetes, Gestational/therapy , Female , Humans , Pregnancy , Risk Factors , Risk Reduction BehaviorABSTRACT
This study aims to describe the native microbiota of fermented spelt, taking into consideration both lactic acid bacteria (LAB) and yeasts, for which little data are available. Five samples of commercial spelt flour were subjected to spontaneous fermentation to obtain a type I sourdough. A total of 186 LAB and 174 yeast isolates were selected at different refreshment steps and subjected to further analyses. Within LAB, coccal isolates constituted 78·5% of the total LAB, with the dominance of Pediococcus pentosaceus. Although documented before as a component, this is the first report of a spelt sourdough fermentation dominated by this homofermentative LAB, characterized by a high acidification rate, ability to utilize a wide range of carbon sources and to grow in high osmolarity conditions. Yeast communities resulted in four dominant species, Saccharomyces cerevisiae, Wickerhamomyces anomalus, Pichia fermentans and Clavispora lusitaniae. This study highlights for the first time the biodiversity and dynamics of yeast communities involved in sourdough fermentation of spelt. Compared to commercial baker's yeast, autochthonous W. anomalus, P. fermentans and S. cerevisiae isolates show a good performance, and their use could be an advantage for their acquired adaptation to the environment, providing stability to the fermentation process. SIGNIFICANCE AND IMPACT OF THE STUDY: Nowadays, there is a renewed interest in products based on spelt. This 'ancient grain' is a highly nutritional grain; however, its use is limited to bread-making processes, which are not standardized. The low baking and sensory quality of spelt can be overcome through fermentation processes. However, the autochthonous microbiota of spelt sourdough is poorly known. This study highlights the dynamics of microbial communities involved in sourdough fermentation of spelt and provides the basis for the selection of autochthonous cultures, with the aim of improving the nutritional potential of spelt and its rheology and bread-making properties.