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Single-layer tungsten disulfide (WS2) is among the most widely investigated two-dimensional materials. Synthesizing it over large areas would enable the exploitation of its appealing optical and electronic properties in industrial applications. However, defects of different nature, concentration and distribution profoundly affect the optical as well as the electronic properties of this crystal. Controlling the defect density distribution can be an effective way to tailor the local dielectric environment and therefore the electronic properties of the system. In this work we investigate the defects in single-layer WS2, grown in different shapes by liquid phase chemical vapor deposition, where the concentration of certain defect species can be controlled by the growth conditions. The properties of the material are surveyed by means of optical spectroscopy, photoelectron spectroscopy and Kelvin probe force microscopy. We determine the chemical nature of the defects and study their influence on the optical and electronic properties of WS2. This work contributes to the understanding of the microscopic nature of the intrinsic defects in WS2, helping the development of defect-based technologies which rely on the control and engineering of defects in dielectric 2D crystals.
ABSTRACT
Polarization and charge transfer strongly characterize the ligand-receptor interaction when metal atoms are present, as for the Au(I)-biscarbene/DNA G-quadruplex complexes. In a previous work (J Comput Aided Mol Des2022, 36, 851-866) we used the ab initio FMO2 method at the RI-MP2/6-31G* level of theory with the PCM [1] solvation approach to calculate the binding energy (ΔEFMO) of two Au(I)-biscarbene derivatives, [Au(9-methylcaffein-8-ylidene)2]+ and [Au(1,3-dimethylbenzimidazole-2-ylidene)2]+, able to interact with DNA G-quadruplex motif. We found that ΔEFMO and ligand-receptor pair interaction energies (EINT) show very large negative values making the direct comparison with experimental data difficult and related this issue to the overestimation of the embedded charge transfer energy between fragments containing metal atoms. In this work, to improve the accuracy of the FMO method for predicting the binding affinity of metal-based ligands interacting with DNA G-quadruplex (Gq), we assess the effect of the following computational features: (i) the electron correlation, considering the Hartree-Fock (HF) and a post-HF method, namely RI-MP2; (ii) the two (FMO2) and three-body (FMO3) approaches; (iii) the basis set size (polarization functions and double-ζ vs. triple-ζ) and (iv) the embedding electrostatic potential (ESP). Moreover, the partial screening method was systematically adopted to simulate the solvent screening effect for each calculation. We found that the use of the ESP computed using the screened point charges for all atoms (ESP-SPTC) has a critical impact on the accuracy of both ΔEFMO and EINT, eliminating the overestimation of charge transfer energy and leading to energy values with magnitude comparable with typical experimental binding energies. With this computational approach, EINT values describe the binding efficiency of metal-based binders to DNA Gq more accurately than ΔEFMO. Therefore, to study the binding process of metal containing systems with the FMO method, the adoption of partial screening solvent method combined with ESP-SPCT should be considered. This computational protocol is suggested for FMO calculations on biological systems containing metals, especially when the adoption of the default ESP treatment leads to questionable results.
Subject(s)
DNA , Quantum Theory , Ligands , SolventsABSTRACT
One of the main challenges of next generation optical communication is to increase the available bandwidth while reducing the size, cost and power consumption of photonic integrated circuits. Graphene has been recently proposed to be integrated with silicon photonics to meet these goals because of its high mobility, fast carrier dynamics and ultra-broadband optical properties. We focus on graphene photodetectors for high speed datacom and telecom applications based on the photo-thermo-electric effect, allowing for direct optical power to voltage conversion, zero dark current, and ultra-fast operation. We report on a chemical vapour deposition graphene photodetector based on the photo-thermoelectric effect, integrated on a silicon waveguide, providing frequency response >65 GHz and optimized to be interfaced to a 50 Ω voltage amplifier for direct voltage amplification. We demonstrate a system test leading to direct detection of 105 Gbit s-1 non-return to zero and 120 Gbit s-1 4-level pulse amplitude modulation optical signals.
ABSTRACT
The employment of two-dimensional materials, as growth substrates or buffer layers, enables the epitaxial growth of layered materials with different crystalline symmetries with a preferential crystalline orientation and the synthesis of heterostructures with a large lattice constant mismatch. In this work, we employ single crystalline graphene to modify the sulfurization dynamics of copper foil for the deterministic synthesis of large-area Cu9S5 crystals. Molecular dynamics simulations using the Reax force-field are used to mimic the sulfurization process of a series of different atomistic systems specifically built to understand the role of graphene during the sulphur atom attack over the Cu(111) surface. Cu9S5 flakes show a flat morphology with an average lateral size of hundreds of micrometers. Cu9S5 presents a direct band-gap of 2.5 eV evaluated with light absorption and light emission spectroscopies. Electrical characterization shows that the Cu9S5 crystals present high p-type doping with a hole mobility of 2 cm2 V-1 s-1.
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Van der Waals heterostructures show many intriguing phenomena including ultrafast charge separation following strong excitonic absorption in the visible spectral range. However, despite the enormous potential for future applications in the field of optoelectronics, the underlying microscopic mechanism remains controversial. Here we use time- and angle-resolved photoemission spectroscopy combined with microscopic many-particle theory to reveal the relevant microscopic charge transfer channels in epitaxial WS_{2}/graphene heterostructures. We find that the timescale for efficient ultrafast charge separation in the material is determined by direct tunneling at those points in the Brillouin zone where WS_{2} and graphene bands cross, while the lifetime of the charge separated transient state is set by defect-assisted tunneling through localized sulphur vacancies. The subtle interplay of intrinsic and defect-related charge transfer channels revealed in the present work can be exploited for the design of highly efficient light harvesting and detecting devices.
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The change in bending rigidity with temperature κ(T) for 2D materials is highly debated: theoretical works predict both increase and decrease. Here we present measurements of κ(T), for a 2D material: AB-stacked bilayer graphene. We obtain κ(T) from phonon dispersion curves measured with helium atom scattering in the temperature range 320-400 K. We find that the bending rigidity increases with temperature. Assuming a linear dependence over the measured temperature region we obtain κ(T)=[(1.3±0.1)+(0.006±0.001)T/K] eV by fitting the data. We discuss this result in the context of existing predictions and room temperature measurements.
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BACKGROUND AND PURPOSE: In patients with Parkinson's disease (PD) with motor fluctuations, total daily OFF time is comprised of both end-of-dose time and the time taken to turn ON with medication. However, little is known about the impact of delays in ON time. METHODS: This was a single-visit pilot study of fluctuating patients with PD attending a routine appointment. During a single visit, adult patients with idiopathic PD who were treated with levodopa for at least 1 year completed a questionnaire evaluating the time waiting for ON and the symptoms experienced while waiting to turn ON. Patients then completed a 5-day home time-to-ON diary, where they documented how long it took to turn ON following their first morning dose of levodopa in 5-min increments. RESULTS: A total of 151 consecutive patients completed the study survey, of whom 97 (64.2%) experienced motor fluctuations. Of the patients experiencing motor fluctuations, 54 (56%) reported delays in ON time (latency >30 min) following their first morning dose of levodopa. Half (51%) reported that they had experienced delayed ON at least once in the previous week and 21% reported having delayed ON during all seven mornings of the previous week. In addition, 10% of patients reported having dose failures on four or more mornings during the previous week. The most common symptoms experienced while waiting for ON were slowness (94.8%), fatigue (87.6%), reduced dexterity (82.5%), problems in walking (66.0%) and problems with balance (59.8%). CONCLUSION: Early-morning OFF problems such as delays in time to ON and dose failures are common in levodopa-treated patients with PD.
Subject(s)
Antiparkinson Agents/administration & dosage , Antiparkinson Agents/therapeutic use , Levodopa/administration & dosage , Levodopa/therapeutic use , Parkinson Disease/drug therapy , Surveys and Questionnaires , Aged , Aged, 80 and over , Appointments and Schedules , Drug Administration Schedule , Female , Humans , Male , Middle Aged , Movement Disorders/drug therapy , Movement Disorders/physiopathology , Pilot Projects , Treatment FailureABSTRACT
The surface structure of Few-Layer Graphene (FLG) epitaxially grown on the C-face of SiC has been investigated by TM-AFM in ambient air and upon interaction with dilute aqueous solutions of bio-organic molecules (l-methionine and dimethyl sulfoxide, DMSO). Before interaction with molecular solutions, we observe nicely ordered, three-fold oriented rippled domains, with a 4.7 ± 0.2 nm periodicity (small periodicity, SP) and a peak-to-valley distance in the range 0.1-0.2 nm. Upon mild interaction with the molecular solution, the ripple periodicity "relaxes" to 6.2 ± 0.2 nm (large periodicity, LP), while the peak-to-valley height increases to 0.2-0.3 nm. When additional energy is transferred to the system through sonication in solution, graphene planes are peeled off, as shown by quantitative analysis of Raman spectroscopy and X-ray photoelectron spectroscopy which indicate a neat reduction of thickness. Upon exfoliation rippled domains are no longer observed. In comparative experiments on cleaved HOPG, we could not observe ripples on pristine samples in ambient air, while LP ripples develop upon interaction with the molecular solutions. Recent literature on similar systems is not univocal regarding the interpretation of rippling. The ensemble of our comparative observations on FLG and HOPG can be hardly rationalized solely on the basis of the surface assembly of molecules, either organic molecules coming from the solution or adventitious species. We propose to consider rippling as the manifestation of the free-energy minimization of quasi-2D layers, eventually affected by factors such as interplanar stacking, and interactions with molecules and/or with the AFM tip.
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One of the major issues in graphene-based optoelectronics is to scale-up high-performing devices. In this work, we report an original approach for the fabrication of efficient optoelectronic devices from scalable tungsten disulfide (WS2)/graphene heterostructures. Our approach allows for the patterned growth of WS2 on graphene and facilitates the realization of ohmic contacts. Photodetectors fabricated with WS2 on epitaxial graphene on silicon carbide (SiC) present, when illuminated with red light, a maximum responsivity R â¼220 A W-1, a detectivity D* â¼2.0 × 109 Jones and a -3 dB bandwidth of 250 Hz. The retrieved detectivity is 3 orders of magnitude higher than that obtained with graphene-only devices at the same wavelength. For shorter illumination wavelengths we observe a persistent photocurrent with a nearly complete charge retention, which originates from deep trap levels in the SiC substrate. This work ultimately demonstrates that WS2/graphene optoelectronic devices with promising performances can be obtained in a scalable manner. Furthermore, by combining wavelength-selective memory, enhanced responsivity and fast detection, this system is of interest for the implementation of 2d-based data storage devices.
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Germanium is emerging as the substrate of choice for the growth of graphene in CMOS-compatible processes. For future application in next generation devices the accurate control over the properties of high-quality graphene synthesized on Ge surfaces, such as number of layers and domain size, is of paramount importance. Here we investigate the role of the process gas flows on the CVD growth of graphene on Ge(100). The quality and morphology of the deposited material is assessed by using µ-Raman spectroscopy, X-ray photoemission spectroscopy, scanning electron microscopy, and atomic force microscopy. We find that by simply varying the carbon precursor flow different growth regimes yielding to graphene nanoribbons, graphene monolayer, and graphene multilayer are established. We identify the growth conditions yielding to a layer-by-layer growth regime and report on the achievement of homogeneous monolayer graphene with an average intensity ratio of 2D and G bands in the Raman map larger than 3.
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Zinc finger protein, FOG2 family member 2 (ZFPM2) (previously named FOG2) gene defects result in the highly morbid congenital diaphragmatic hernia (CDH) in humans and animal models. In a cohort of 275 CDH patient exomes, we estimated the prevalence of damaging ZFPM2 mutations to be almost 5%. Genetic analysis of a multigenerational family identified a heritable intragenic ZFPM2 deletion with an estimated penetrance of 37.5%, which has important implications for genetic counseling. Similarly, a low penetrance ZFPM2 frameshift mutation was observed in a second multiplex family. Isolated CDH was the predominant phenotype observed in our ZFPM2 mutation patients. Findings from the patients described herein indicate that ZFPM2 point mutations or deletions are a recurring cause of CDH.
Subject(s)
DNA-Binding Proteins/genetics , Hernias, Diaphragmatic, Congenital/epidemiology , Hernias, Diaphragmatic, Congenital/genetics , Mutation/genetics , Phenotype , Transcription Factors/genetics , Base Sequence , Cohort Studies , DNA Copy Number Variations , Exome/genetics , Hernias, Diaphragmatic, Congenital/pathology , Humans , Molecular Sequence Data , Penetrance , Prevalence , Sequence Analysis, DNAABSTRACT
UNLABELLED: In elderly subjects, past researches have already underlined the role of nutritional status as a basic factor able to influence the prognosis either in acute wards or in rehabilitation and long-term care settings. Aim of the study is that of retrospectively verify, through a multivariate analysis, the factors able to condition mortality in long-term care, paying particular attention to the nutritional status. METHODS: The survey included 513 patients aged more than 65 years admitted to a long-term care unit during a three years period. Exitus within the first three months of hospitalization was considered the outcome variable, while baseline functional, cognitive, clinical and nutritional status were considered the independent variables eventually related to mortality. RESULTS: The univariate analysis found that some variables were significantly correlated with the outcome: comorbidity, ADL, cognitive status, pressure sores, albumin, transferrin, CRP, mucoprotein, cholesterol, cholinesterase, MAMC and MNA. The predictive value of the block model of the logistic regression analysis was 77.9% (specificity = 85.3%, sensitivity = 63.9%). With the forward stepwise analysis only MNA, cholinesterase, CRP and mucoprotein were considered in the final model. In this case the predictive value of the model was 79.3% (specificity = 84.6%, sensitivity = 69.46%).
Subject(s)
Geriatric Assessment , Hospitalization , Long-Term Care , Malnutrition/mortality , Nutrition Assessment , Nutritional Status , Activities of Daily Living , Aged , Aged, 80 and over , Biomarkers/blood , C-Reactive Protein/metabolism , Cholinesterases/blood , Cognition , Comorbidity , Female , Glycoproteins/blood , Health Care Surveys , Housing for the Elderly , Humans , Logistic Models , Male , Multivariate Analysis , Predictive Value of Tests , Prognosis , Retrospective Studies , Risk FactorsABSTRACT
Obesity is a prevalent health disease among the elderly as it contributes to the early onset of chronic morbidity and functional impairment and is also related to premature mortality. The prevalence of sarcopenic-obesity increases too with age in each sex leading to a significantly higher prevalence of physical impairment and disability, as well as higher prevalence of metabolic syndrome. We observe a natural phenomenon (ageing) and a complex world-wide illness (obesity) that should not be merely treated as the sum of the treatments for the elderly and for the obese. The balance between the potential benefits of treatment interventions, reducing premature morbidity and mortality, and the impact on quality of life in old age may be different from young and adult age in case of obesity and need to be seriously considered.
Subject(s)
Aging , Metabolic Syndrome/etiology , Obesity , Quality of Life , Aged , Aged, 80 and over , Body Mass Index , Female , Humans , Interdisciplinary Communication , Italy/epidemiology , Male , Metabolic Syndrome/epidemiology , Metabolic Syndrome/prevention & control , Obesity/complications , Obesity/epidemiology , Obesity/etiology , Obesity/physiopathology , Obesity/therapy , Prevalence , Risk Factors , Sarcopenia/etiologyABSTRACT
UNLABELLED: Obesity, associated with morbidity and mortality, is a complex disorder, characterised by an increase in fat mass (FM). Most authors agree in considering essential an integrated treatment made up of nutritional intervention, physical reconditioning programme and cognitive-behavioural psychotherapy. However, the feasibility is problematic and data in literature confirming the validity of this approach are poor. AIM: To verify the efficacy of a multidimensional approach (Nutritional Psycho-Physical Reconditioning - NPPR) in obesity treatment. METHODS: All patients admitted from June 2002 to June 2004 (464 subjects) ranged from 18 to 65 years old, with a body mass index (BMI) >30 kg/m2 were included in the programme. After the nutritional status evaluation a standard dietetic treatment (group N) or an integrated and multidisciplinary obesity treatment (group NPPR) was proposed. RESULTS: In group NPPR treatment duration was significantly higher (142.6+/-26 vs 48.6+/-55 days - p=0.000), while the drop-out amount was definitely lower (5.5 vs 54.4%; p=0.000). Weight loss compared to the initial weight and the difference between initial and final FM resulted significantly higher in group NNPR. Subjects in NPPR obtained a higher increase in the distance covered in a 6-minute walk test (59.9+/-19 vs 40.5+/-17 m; p=0.04) and in muscular strength. State and trait anxiety, mood and quality of life scores improved in NPPR subjects while remained substantially stable in group N. CONCLUSIONS: An integrated approach to obesity is the way to be pursued in order to obtain important and at least short-term results.
Subject(s)
Anti-Obesity Agents/therapeutic use , Cognitive Behavioral Therapy , Diet, Reducing , Interdisciplinary Communication , Obesity/therapy , Patient Care Team , Adult , Aged , Body Mass Index , Delivery of Health Care, Integrated , Female , Humans , Male , Middle Aged , Nutritional Requirements , Nutritional Status , Nutritive Value , Obesity/diet therapy , Obesity/drug therapy , Obesity/psychology , Treatment Outcome , Weight Loss , Young AdultABSTRACT
Quasi-free-standing epitaxial graphene is obtained on SiC(0001) by hydrogen intercalation. The hydrogen moves between the (6 square root(3) x 6 square root(3))R30 degrees reconstructed initial carbon layer and the SiC substrate. The topmost Si atoms which for epitaxial graphene are covalently bound to this buffer layer, are now saturated by hydrogen bonds. The buffer layer is turned into a quasi-free-standing graphene monolayer with its typical linear pi bands. Similarly, epitaxial monolayer graphene turns into a decoupled bilayer. The intercalation is stable in air and can be reversed by annealing to around 900 degrees C.
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BACKGROUND: Malnutrition due to undernutrition or overnutrition is highly prevalent in hospital in-patients and it decisively conditions patients clinical outcome. One of the most influencing factors of malnutrition in hospitalized patients is--at least in part--the Catering Service Quality. AIM: Is to verify, over a 5 year period, the course of the quality of the institutional Catering Service, verifying the effectiveness of the quality improvement process used. METHODS: Quality control was performed by objective (meal order accuracy, proper distribution of food in trolleys, route time from the kitchen to the ward and time of food distribution, food weight and temperature, waste assessment) and subjective assessment (quality was measured by giving the patients a questionnaire after meals). RESULTS: The survey included: 572 meals and 591 interviews. A significant amount of "qualitative" errors (lack of respect for patient preferences or at the moment of supplying the food trolley) have been found. Over the time and the amount of patients that wasted a considerable amount of the portion served was considerably reduced food temperature have been improved. Also patient satisfaction with menu variability, portion size, temperature and cooking quality improved over time. The overall ratings of meals under observation improved too in fact, positive opinions ranged from 18% in 2002 to 48.3% in 2006. CONCLUSION: Ongoing research and quality verification, which include all catering service workers, yields a constant improvement in quality. Patients in healthcare settings should receive a service they appreciates, but it should be--at the same time--correct from a nutritional point of view. For this reason, it is necessary a continuous mediation between customers satisfaction and nutritionists work, dieticians and nursing staff. From this point of view the educational approach becomes essential to feed patient compliance to dietetic treatment that will continue after discharge.
Subject(s)
Food Handling/methods , Food Handling/standards , Food Service, Hospital/standards , Food/standards , Patient Satisfaction , Quality Control , Aged , Female , Humans , Length of Stay , Male , Menu Planning , Middle Aged , Taste , TemperatureABSTRACT
Crystalline silicon carbide (SiC) and silicon (Si) biocompatibility was evaluated by directly culturing three mammalian cell lines on these semiconducting substrates. Cell proliferation and adhesion quality were studied using MTT [3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide] assays and fluorescent microscopy. The reported results show that SiC is indeed a more biocompatible substrate than Si. The surface wettability of SiC and Si samples was evaluated through static contact angle measurements, which provided interesting information regarding the influence of different cleaning procedures on the SiC surfaces. The cell proliferation data are discussed in light of the contact angle measurements results. This joint analysis leads to interesting conclusions that may help to uncover the main factors that define a semiconductor's biocompatibility.
Subject(s)
Biocompatible Materials/administration & dosage , Biocompatible Materials/chemistry , Carbon Compounds, Inorganic/chemistry , Cell Survival/drug effects , Silicon Compounds/chemistry , Silicon/chemistry , Animals , Cell Line , Crystallization/methods , Humans , Materials Testing , Mice , WettabilityABSTRACT
BACKGROUND AND PURPOSE: Thioredoxin (Trx) is an oxidoreductase that prevents free radical-induced cell death in cultured cells. Here we assessed the mechanism(s) underlying the cardioprotective effects of Trx in vivo. EXPERIMENTAL APPROACH: The effects of myocardial ischemia (30 min) and reperfusion were measured in mice, with assays of myocardial apoptosis, superoxide production, NOx and nitrotyrosine content, and myocardial infarct size. Recombinant human Trx (rhTrx, 0.7-20 mg kg(-1), i.p.) was given 10 min before reperfusion. KEY RESULTS: Treatment with 2 mg kg(-1) rhTrx significantly decreased myocardial apoptosis and reduced infarct size (P<0.01). Nitrotyrosine content of cardiomyocytes was markedly reduced in rhTrx-treated animals (P<0.01). To further identify the mechanisms by which rhTrx may exert its anti-nitrative effect, iNOS expression and production of NOx and superoxide were determined. Treatment with rhTrx had no significant effect on iNOS expression or NOx content in the ischemic/reperfused heart. However, it markedly upregulated mSOD and reduced tissue superoxide content. To further establish a causative link between the anti- peroxynitrite effect and the cardioprotective effect of rhTrx, cultured adult cardiomyocytes were incubated with SIN-1, a peroxynitrite donor, (50 microM for 3 h) resulting in a nitrotyrosine content comparable to that seen in the ischemic/reperfused heart and causing significant cardiomyocyte apoptosis (P<0.01). Treatment with rhTrx markedly decreased SIN-1 induced apoptosis (P<0.01). CONCLUSIONS AND IMPLICATIONS: These results demonstrate that Trx is a novel anti-apoptotic and cardioprotective molecule that exerts its cardioprotective effects by reducing ischemia/reperfusion-induced oxidative/nitrative stress.
Subject(s)
Apoptosis/drug effects , Myocardial Ischemia/drug therapy , Myocardium/pathology , Nitric Oxide/biosynthesis , Oxidative Stress/drug effects , Thioredoxins/pharmacology , Animals , Male , Mice , Molsidomine/analogs & derivatives , Molsidomine/pharmacology , Myocardial Ischemia/pathology , Myocytes, Cardiac/drug effects , Myocytes, Cardiac/pathology , Peroxynitrous Acid/metabolism , Superoxides/metabolism , Tyrosine/analogs & derivatives , Tyrosine/analysisABSTRACT
The achievement of extensive and meaningful molecular dynamics simulations requires both the detailed knowledge of the basic features of the intermolecular interaction and the representation of the involved potential energy surface in a simple, natural and analytical form. This double request stimulated us to extend to ion-molecule systems a semiempirical method previously introduced for the description of weakly interacting atom-molecule aggregates and formulated in terms of atomic species-molecular bond interaction additivity. The method is here applied to the investigation of the prototypical M(+)-C6H6 systems (M = Li, Na, K, Rb and Cs) and some of its predictions are tested against accurate ab initio calculations. Such calculations have been performed by employing the MP2 method and large basis sets, privileging the description of the metal atoms. The agreement between potential energy scans semiempirically obtained and ab initio results is good for all the investigated geometries, thus showing that the adopted representation is in general able to reproduce all the main features of the potential energy surface for these systems. The role of the various noncovalent interaction components, as a function of the geometry and of the intermolecular distance in the M(+)-C6H6 complexes, is also investigated for a more detailed assessment of the results of the semiempirical method.
Subject(s)
Benzene/chemistry , Cations/chemistry , Computer Simulation , Hydrogen Bonding , Kinetics , Models, Molecular , Molecular Conformation , Molecular Structure , ThermodynamicsABSTRACT
Studies on scalp hair from psoriatic lesions have revealed marked irregularities in the cuticular pattern. The aim of this study was to investigate the incidence of hair shaft disorders in psoriatic patients and to evaluate the possibility of a correlation with scalp involvement. We examined hair from 39 psoriatic patients using scanning electron microscopy and compared it with hair from a control group of 12 healthy people. We confined our observations of the hair fibres to the areas nearest the root. Our data confirm previous observations indicating that dystrophic changes in hair cuticle cells occur more often in hairs from both unaffected and affected skin of psoriatic patients compared with normal subjects. No differences were observed between hair shafts taken from affected and unaffected psoriatic areas; cuticular breakage and an abraded cuticular surface were present only in the hair of psoriatic patients.