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1.
J Chem Phys ; 160(24)2024 Jun 28.
Article in English | MEDLINE | ID: mdl-38920401

ABSTRACT

Lead halide perovskites (LHPs) have gained prominence for their exceptional photophysical properties, holding promise for applications in high-end optoelectronic devices. However, the presence of lead is one of the major obstacles to the commercialization of LHPs in the field of photovoltaics. To address this, researchers have explored environment friendly lead-free perovskite solar cells by investigating non-toxic perovskite materials. This study explores the enhancement of photophysical properties through chemical engineering, specifically cation exchange, focusing on the crucial photophysical process of hot carrier cooling. Employing femtosecond transient absorption spectroscopy and optical pump terahertz probe spectroscopy, we have probed the carrier relaxation dynamics in A3Sb2I9 with cesium and rubidium cations. This study unravels that the carrier relaxation is found to be slower in Rb3Sb2I9; along with this, the transient mobility decay is found to be retarded. Overall, this study suggests that an antimony-based Rb3Sb2I9 perovskite could be a substantial lead-free perovskite in photovoltaics. These findings provide valuable insights into cation engineering strategies, aiming to improve the overall performance of lead-free-based photovoltaic devices.

2.
J Phys Chem Lett ; 15(25): 6575-6584, 2024 Jun 27.
Article in English | MEDLINE | ID: mdl-38885443

ABSTRACT

Lead-free double perovskite nanocrystals (A2B'(III)B″(I)X6 NCs) address the instability and toxicity concerns of lead-based counterparts, but their device performance is limited by subpar absorption and unexplored carrier dynamics. Impurity ion doping offers a route to tune electrical conductivity and charge carrier transport. Herein, we synthesized Cu-doped Cs2AgBiBr6 (CABB) nanocrystals using a hot-injection approach and investigated the charge carrier's dynamics through ultrafast pump-probe spectroscopy. Copper introduction into the CABB lattice enhanced absorption in the near-infrared region and introduced sub-band gap defect states in CABB NCs. The transient absorption study revealed a faster bleach decay with increased copper doping, as a result of charge transfer from the conduction band to copper defect states. Also, an optical pump terahertz probe study displays higher photoconductivity and mobility in Cu-doped CABB NCs. Slower mobility decay in Cu-doped systems was attributed to the charge carrier's entrapment at the defect state. These findings suggest that copper-doped CABB is a superior contender for optoelectronic applications over conventional CABB.

3.
Nanoscale ; 15(34): 14081-14092, 2023 Sep 01.
Article in English | MEDLINE | ID: mdl-37581308

ABSTRACT

Advancements in photovoltaic research suggest that tin-based perovskites are potential alternatives to traditional lead-based structures. Cs2SnI6, specifically, stands out as a notable candidate, exhibiting impressive performance. However, its complete potential remains untapped primarily owing to the limited understanding of its photophysics. In light of this, this study aims to bridge this knowledge gap. To commence our study, we first executed theoretical investigations to locate the energetically diverse excitons within the Brillouin zone. Building on this knowledge, we then utilized transient absorption spectroscopy to investigate their temporal evolution. Herein, we observed the formation of high-energy excitons even when the incident photon energy was below the necessary threshold, which is quite distinctive and intriguing. Of particular interest is the generation of ultraviolet (UV) domain exciton using visible photons, which implies that Cs2SnI6 has the potential for efficient solar light harvesting. Tracking the kinetics revealed that this unique finding arises due to the intertwined formation and decay pathways undertaken by the different excitons, aided by intervalley scattering and phonon absorption processes. In addition, we found that the decay of the UV exciton was unusually slow. Transient mobility investigations were undertaken to probe the carrier transport behavior that further established hot carriers (HCs) in Cs2SnI6 to be highly mobile and susceptible to polaron formation. Overall, our findings demonstrate that Cs2SnI6 is a strong candidate for HC-based photovoltaics because it possesses all the prerequisites desired for such applications.

4.
Angew Chem Int Ed Engl ; 62(31): e202308034, 2023 Aug 01.
Article in English | MEDLINE | ID: mdl-37332091

ABSTRACT

We demonstrate direct evidence of photoinduced through-space intervalence charge transfer (IVCT) between two cofacially arranged redox-active pairs in metal-organic frameworks and their dynamic variation with their molecular separation. Two homologous MOFs [Co2 (NDC)2 (DPTTZ)2 ]. DPTTZ. DMF, 1 and [Co2 (BDC)2 (DPTTZ)2 ]. DMF, 2 (where NDC=naphthalene dicarboxylate, BDC=benzene dicarboxylate, DPTTZ=N, N'-di(4-pyridyl)thiazolo-[5,4-d]thiazole, DMF=N, N'-dimethyl formamide) are considered for this, whose intra-dimer distance of redox-active DPTTZ ligands differs ca. 1 Šfrom one system to another. Spectroelectrochemical study detects the formation of IVCT band at the NIR region between cofacially oriented DPTTZ molecules in both MOFs. Transient spectroscopy shows faster charge separation as well as charge recombination when intra-dimer distance is lesser (in MOF 2) due to stronger electronic coupling. We quantify the extent of IVCT by charge transfer integral calculation; and also by optical pump terahertz probe spectroscopy, where MOF 2 shows three times higher carrier mobility due to lesser inter-DPTTZ distance than MOF 1. These findings reveal a more localized aspect of through-space IVCT between cofacially organized redox-active pair in a three-dimensional framework.

5.
Chem Commun (Camb) ; 58(100): 13899-13902, 2022 Dec 15.
Article in English | MEDLINE | ID: mdl-36454083

ABSTRACT

A temperature dependent transient absorption study has been demonstrated for Mn2+ doped CsPbBr3 nanoplatelets. At 5 K, charge transfer is suppressed due to the trapping of charge carriers in defect states. By contrast, at 300 K, an efficient charge/energy transfer process is observed as the thermally active carriers become de-trapped from the defect states upon strong exciton-phonon coupling.

6.
J Phys Chem Lett ; 13(48): 11354-11362, 2022 Dec 08.
Article in English | MEDLINE | ID: mdl-36454185

ABSTRACT

Utilization of hot carriers is very crucial in improving the efficiency of solar energy devices. In this work, we have fabricated an Sb2Se3/CdSe p-n heterojunction via a cation exchange method and investigated the possibility of hot electron transfer and relaxation pathways through ultrafast spectroscopy. The enhanced intensity of the CdSe hot excitonic (1P) bleach in the heterostructure system confirmed the hot electron transfer from Sb2Se3 to CdSe. Both the 1S and 1P signals are dynamically very slow in the heterosystem, validating this charge migration phenomenon. Interestingly, recovery of the 1P signal is much slower than that of 1S. This is very unusual as 1S is the lowest-energy state. This observation indicates the strength of hot electron transfer in this unique heterojunction, which helps in increasing the carrier lifetime in the hot state. Extended separation of charge carriers and enhanced hot carrier lifetime would be extremely helpful in extracting carriers and boost the performance of optoelectronic devices.

7.
J Cancer Res Ther ; 18(6): 1541-1547, 2022.
Article in English | MEDLINE | ID: mdl-36412407

ABSTRACT

Introduction: The aim of this study was to compare overtreatment rates of see and treat colposcopy-based single step protocol with cytology and colposcopy-guided biopsy-based conventional three-step protocol using loop electrosurgical excision procedure (LEEP) for treatment of preinvasive lesions of cervix. Materials and Methods: Prospective interventional study was carried out over a period of 1 year. Recruitment of cases was done from the 664 diagnostic colposcopies performed for various gynecological indications. Among 496 colposcopies performed exclusively for unhealthy cervix on per speculum examination, 74 women had high-grade colposcopy (Swede score ≥5). Subsequently, 50 women were enrolled under the see and treat arm, arm 1 and underwent LEEP. In study arm 2, conventional three-step strategy, concurrently 22 women with abnormal cytology. ≥ Atypical squamous cells of undetermined significance and unhealthy cervix were enrolled for colposcopy and if indicated, guided biopsy was obtained and tissue was sent for histopathology. Only 12 such women having HPE reports of cervical intraepithelial neoplasia (CIN) 2 or 3 were subjected to LEEP. Overtreatment was defined as CIN 1 or less on final LEEP tissue histopathology. Results: The overtreatment rate in See and Treat protocol was 44% when colposcopy Swede score cutoff was considered 5, which fell down to 0% when Swede score cutoff was taken 7. Conventional three step protocol had an overtreatment rate of 8.3%. Incidentally diagnosed high-grade CIN or invasive cancer was found in 24%. Discrepancy between biopsy tissue and LEEP tissue histopathology was 50% in conventional arm. Conclusion: Women with unhealthy cervix having high-grade colposcopy (Swede score ≥7) can be directly subjected to LEEP without waiting for results of any initial screening modality. Advantages include minimal over treatment coupled with reduced patient visits and interventions.


Subject(s)
Uterine Cervical Dysplasia , Uterine Cervical Neoplasms , Female , Humans , Pregnancy , Electrosurgery/methods , Uterine Cervical Neoplasms/diagnosis , Uterine Cervical Neoplasms/surgery , Uterine Cervical Neoplasms/pathology , Prospective Studies , Colposcopy , Uterine Cervical Dysplasia/diagnosis , Uterine Cervical Dysplasia/surgery , Uterine Cervical Dysplasia/pathology
8.
Int J Appl Basic Med Res ; 12(3): 177-184, 2022.
Article in English | MEDLINE | ID: mdl-36131854

ABSTRACT

Objective: The aim of this study was to evaluate the predictive value of Immunohistochemical p53 cut-off scores as an adjunct to routine histopathology for better diagnosis of cervical lesions. Materials and Methods: Prospective study carried out for 1 year. After ethical approval and informed consent, a total of 100 cervical tissue samples were analyzed; chronic cervicitis (CC)-15, cervical intraepithelial neoplasia (CIN)-40, and squamous cell carcinoma cervix (SCC)-45 (FIGO 2018 clinical staging). After routine processing of tissue specimen, hematoxylin and eosin (HE) staining was done. Grading of cervical precancerous lesions (CIN) was done as per World Health Organisation criteria as CIN 1,2 or 3. Broder's grading was assigned for every SCC sample. Results: Mean p53 scores of CC, CIN, and SCC cases were 0.0, 1.70, and 4.38, respectively, CIN 1, 2, and 3 were 1.07, 1.63, and 2.22, respectively. SCC was differentiated from CIN3 with p53 ≥4.5 as predictor for SCC, sensitivity and specificity were 57.8% and 88.9%, respectively. Overall diagnostic accuracy of the proposed scoring system for differentiating CC, CIN, and SCC was 61%, while the accuracy of previous methods of interpreting p53 immunoreactivity as immunoscore >2 or arbitrary cut-off of >10% cells with nuclear positivity was only 48%. Conclusion: ROC-derived immunoscore cut-offs can provide the much-needed objectivity and optimal decision thresholds to immunohistochemistry interpretation.

9.
Nanotechnology ; 33(48)2022 Sep 15.
Article in English | MEDLINE | ID: mdl-35785756

ABSTRACT

Lead-free halide-based double perovskites (DPs) have established themselves as the emerging nontoxic alternatives for photovoltaic (PV) applications thus substituting the long-standing lead halide perovskites. Among the prospective lead-free DPs, Cs2AgBiBr6has gained immense popularity owing to the fascinating properties demonstrated by them including low carrier effective mass and microsecond lifetime for electron-hole recombination. Nevertheless, the large, indirect bandgap remains the prime hurdle that restrains commercialization of the Cs2AgBiBr6DPs based PV devices. A rational solution could be designing its heterostructure with another suitable material that could mitigate the inadequacies of Cs2AgBiBr6DPs. With this line of thought, herein we synthesized a composite of Cs2AgBiBr6DPs with CdSe NCs and then performed transient absorption (TA) spectroscopic measurements to introspect its photophysical aspects. Executing excitation energy-dependent studies clearly reveal the carrier transfer efficiency to be strongly pump-dependent. Upon exciting with 350 nm pump, in compliance with the energy band alignment and tendency of both the constituents to be photoexcited across their bandgap, there is a bidirectional transfer of hot electrons anticipated in the composite system. Nevertheless, the TA outcomes indicate the transfer of hot electrons from CdSe to Cs2AgBiBr6to be more favorable out of the bidirectional pathways. Employing further lower pump energies (480 nm) when only CdSe NCs are capable of being excited, the transfer efficiency of the electrons from CdSe to Cs2AgBiBr6is noticed to be fairly low. Besides this, when the pump wavelength is tuned to 530 nm i.e. quite close to the CdSe band edge, no electron transfer is noticeable despite the anticipation from thermodynamic feasibility. Thus, as reflected by the TA kinetics, electron transfer is discerned to be more efficient from the hot states rather than the band edges. Most advantageously, charge separation is successfully achieved in this never explored composite architecture which eases the carrier extraction and minimizes the otherwise prevalent fast recombination processes.

10.
Chem Rec ; 22(11): e202200106, 2022 Nov.
Article in English | MEDLINE | ID: mdl-35882519

ABSTRACT

Hot carrier extraction-based devices are presently being persuaded as the most revolutionary means of surpassing the theoretical thermodynamic conversion efficiency limit (∼67 % for a model hot carrier solar cell). However, for practical realisation, there stand various hurdles that need to be surmounted, a major among all being the rapid hot carrier cooling rate. Though, the perovskite family has already demonstrated itself to exhibit slower cooling in contrast to the prototypical semiconductors. Decelerating this entire process of cooling further can prove to be a crucial stride in this regard. Quite contrarily, for the optoelectronic applications the situation is entirely conflicting where quick rate of cooling is a chief prerequisite. In the recent times, there have been various key developments that have targeted altering this cooling rate by various chemically engineered strategies. This review highlights such blueprints that can be utilized towards the advantageous alteration of the carrier cooling in accordance with the device requirements.

11.
Hum Brain Mapp ; 43(12): 3809-3823, 2022 08 15.
Article in English | MEDLINE | ID: mdl-35467058

ABSTRACT

In the largest sample studied to date, white matter microstructural trajectories and their relation to persistent symptoms were examined after pediatric mild traumatic brain injury (mTBI). This prospective, longitudinal cohort study recruited children aged 8-16.99 years with mTBI or mild orthopedic injury (OI) from five pediatric emergency departments. Children's pre-injury and 1-month post-injury symptom ratings were used to classify mTBI with or without persistent symptoms. Children completed diffusion-weighted imaging at post-acute (2-33 days post-injury) and chronic (3 or 6 months via random assignment) post-injury assessments. Mean diffusivity (MD) and fractional anisotropy (FA) were derived for 18 white matter tracts in 560 children (362 mTBI/198 OI), 407 with longitudinal data. Superior longitudinal fasciculus FA was higher in mTBI without persistent symptoms relative to OI, d (95% confidence interval) = 0.31 to 0.37 (0.02, 0.68), across time. In younger children, MD of the anterior thalamic radiations was higher in mTBI with persistent symptoms relative to both mTBI without persistent symptoms, 1.43 (0.59, 2.27), and OI, 1.94 (1.07, 2.81). MD of the arcuate fasciculus, -0.58 (-1.04, -0.11), and superior longitudinal fasciculus, -0.49 (-0.90, -0.09) was lower in mTBI without persistent symptoms relative to OI at 6 months post-injury. White matter microstructural changes suggesting neuroinflammation and axonal swelling occurred chronically and continued 6 months post injury in children with mTBI, especially in younger children with persistent symptoms, relative to OI. White matter microstructure appears more organized in children without persistent symptoms, consistent with their better clinical outcomes.


Subject(s)
Brain Concussion , White Matter , Brain/diagnostic imaging , Brain Concussion/diagnostic imaging , Child , Diffusion Tensor Imaging/methods , Humans , Longitudinal Studies , Prospective Studies , White Matter/diagnostic imaging
12.
J Phys Chem Lett ; 13(1): 83-90, 2022 Jan 13.
Article in English | MEDLINE | ID: mdl-34958589

ABSTRACT

Rare-earth ion (RE3+) doping in cesium lead chloride (CsPbCl3) has unlocked novel prospects to explore changes in optical, magnetic, and charge carrier transport properties. This leads to a huge advancement in optoelectronic applications, yet deep understanding of the photophysics governing the energy transfer processes is lacking and demands vital attention. Herein, we probe into the mechanistic transfer processes from the band edge of the host (CsPbCl3) to the dopant europium ion (Eu3+) with the aid of femtosecond fluorescence upconversion and transient absorption (TA) spectroscopy. The upconversion measurement portrays a defect-mediated cascading energy transfer from CsPbCl3 to Eu3+ and further cross-relaxation among Eu3+ states. Moreover, TA studies reveal that there is charge transfer from the band edge of CsPbCl3 to doping-induced shallow defect states. Furthermore, two-photon absorption study establishes no compromise in the transfer mechanism even upon bandgap excitation. This work validates that Eu-CsPbCl3 is an apt entrant for optoelectronic applications.

13.
Brain Imaging Behav ; 16(3): 991-1002, 2022 Jun.
Article in English | MEDLINE | ID: mdl-34694520

ABSTRACT

Motion can compromise image quality and confound results, especially in pediatric research. This study evaluated qualitative and quantitative approaches to motion artifacts detection and correction, and whether motion artifacts relate to injury history, age, or sex in children with mild traumatic brain injury or orthopedic injury relative to typically developing children. The concordance between qualitative and quantitative motion ratings was also examined. Children aged 8-16 years with mild traumatic brain injury (n = 141) or orthopedic injury (n = 73) were recruited from the emergency department and completed an MRI scan roughly 2 weeks post-injury. Typically developing children (n = 41) completed a single MRI scan. T1- and diffusion-weighted images were visually inspected and rated for motion artifacts by trained examiners. Quantitative estimates of motion artifacts were derived from FreeSurfer and FSL. Age (younger > older) and sex (boys > girls) were significantly associated with motion artifacts on both T1- and diffusion-weighted images. Children with mild traumatic brain or orthopedic injury had significantly more motion-corrupted diffusion-weighted volumes than typically developing children, but mild traumatic brain injury and orthopedic injury groups did not differ from each other. The exclusion of motion-corrupted volumes did not significantly change diffusion tensor imaging metrics. Results indicate that automated quantitative estimates of motion artifacts, which are less labour-intensive than manual methods, are appropriate. Results have implications for the reliability of structural MRI research and highlight the importance of considering motion artifacts in studies of pediatric mild traumatic brain injury.


Subject(s)
Artifacts , Brain Concussion , Brain/diagnostic imaging , Brain/pathology , Brain Concussion/diagnostic imaging , Brain Concussion/pathology , Child , Diffusion Tensor Imaging/methods , Female , Humans , Magnetic Resonance Imaging/methods , Male , Motion , Reproducibility of Results
14.
Neuroimage Clin ; 32: 102887, 2021.
Article in English | MEDLINE | ID: mdl-34911193

ABSTRACT

BACKGROUND: Pediatric mild traumatic brain injury (mTBI) affects millions of children annually. Diffusion tensor imaging (DTI) is sensitive to axonal injuries and white matter microstructure and has been used to characterize the brain changes associated with mild traumatic brain injury (mTBI). Neurite orientation dispersion and density imaging (NODDI) is a diffusion model that can provide additional insight beyond traditional DTI metrics, but has not been examined in pediatric mTBI. The goal of this study was to employ DTI and NODDI to gain added insight into white matter alterations in children with mTBI compared to children with mild orthopedic injury (OI). METHODS: Children (mTBI n = 320, OI n = 176) aged 8-16.99 years (12.39 ± 2.32 years) were recruited from emergency departments at five hospitals across Canada and underwent 3 T MRI on average 11 days post-injury. DTI and NODDI metrics were calculated for seven major white matter tracts and compared between groups using univariate analysis of covariance controlling for age, sex, and scanner type. False discovery rate (FDR) was used to correct for multiple comparisons. RESULTS: Univariate analysis revealed no significant group main effects or interactions in DTI or NODDI metrics. Fractional anisotropy and neurite density index in all tracts exhibited a significant positive association with age and mean diffusivity in all tracts exhibited a significant negative association with age in the whole sample. CONCLUSIONS: Overall, there were no significant differences between mTBI and OI groups in brain white matter microstructure from either DTI or NODDI in the seven tracts. This indicates that mTBI is associated with relatively minor white matter differences, if any, at the post-acute stage. Brain differences may evolve at later stages of injury, so longitudinal studies with long-term follow-up are needed.


Subject(s)
Brain Concussion , White Matter , Brain/diagnostic imaging , Brain Concussion/diagnostic imaging , Child , Diffusion Tensor Imaging , Humans , Neurites , White Matter/diagnostic imaging
15.
J Phys Chem Lett ; 12(49): 11865-11872, 2021 Dec 16.
Article in English | MEDLINE | ID: mdl-34874742

ABSTRACT

Comprehensive understanding of charge carrier dynamics in the heterostructure based photocatalytic materials will strengthen their candidature as future solar energy harvesting resources. Here, in this work, the g-C3N4(CN)/ZnIn2S4 (ZIS) heterostructure was successfully synthesized and a direct spectroscopic correlation was established between excited-state charge carrier dynamics and enhanced photocatalytic activity using ultrafast transient absorption (TA) spectroscopy. TA analysis demonstrated the dominance of hot electron transfer over the band edge one. The photogenerated hot electrons migrated from the high-energy excitonic states of CN toward ZIS in the subpicosecond time scale. Broad-band (UV to NIR) ultrafast transient pump-probe spectroscopy revealed the collective effect of hot electron transfer as well as trap-state mediated electron delocalization in the enhanced photocatalytic H2 evolution. This work reveals the role of photogenerated carriers in the photocatalytic performance of the CN/ZIS heterostructure and would create a new avenue toward the advancement of CN based heterostructure in photocatalytic devices.

16.
J Phys Chem Lett ; 12(45): 10958-10968, 2021 Nov 18.
Article in English | MEDLINE | ID: mdl-34738822

ABSTRACT

Tin chalcogenides (SnX, X = S, Se)-based heterostructures (HSs) are promising materials for the construction of low-cost optoelectronic devices. Here, we report the synthesis of a SnSe/CdSe HS using the controlled cation exchange reaction. The (400) plane of SnSe and the (111) plane of CdSe confirm the formation of an interface between SnSe and CdSe. The Type I band alignment is estimated for the SnSe/CdSe HS with a small conduction band offset (CBO) of 0.72 eV through cyclic voltammetry measurements. Transient absorption (TA) studies demonstrate a drastic enhancement of the CdSe biexciton signal that points toward the hot carrier transfer from SnSe to CdSe in a short time scale. The fast growth and recovery of CdSe bleach in the presence of SnSe indicate charge transfer back to SnSe. The observed delocalization of carriers in these two systems is crucial for an optoelectronic device. Our findings provide new insights into the fabrication of cost-effective photovoltaic devices based on SnSe-based heterostructures.

17.
J Phys Chem Lett ; 12(20): 5000-5008, 2021 May 27.
Article in English | MEDLINE | ID: mdl-34018752

ABSTRACT

Elemental doping has already been established to be one of the most effective approaches for band-gap engineering and controlled material response for improved photocatalytic activity. Herein atomically thin ZnIn2S4 (ZIS) nanosheets were doped with O and N separately, and the effects of doping were spectroscopically investigated for photocatalytic H2 evolution. Steady-state photoluminescence studies revealed an enhanced charge-carrier population in the doped systems along with a defect-state-induced broad peak in the red region of the spectra. Transient absorption (TA) spectroscopy demonstrated that the conduction-band-edge electrons are transferred on an ultrafast time scale to the inter-band-gap defect states. TA analysis suggests that O and N doping contributes to the defect state concentration and ensures an enhanced photocatalytic activity of the system. This detailed spectroscopic analysis uncovers the role of inter-band-gap defect states in the photocatalytic activity of ZIS and will open new avenues for the construction of nanosheet-based optical devices.

18.
Psychiatry Res Neuroimaging ; 308: 111236, 2021 02 28.
Article in English | MEDLINE | ID: mdl-33340961

ABSTRACT

Absence of insight owing to impaired self-reflection and lack of touch with reality is a hallmark of schizophrenia. Functional imaging studies in healthy individuals have implicated the frontal pole (FP), sub-division of the prefrontal cortex in self-reflective processes. Despite the significance of self-referential processing in the pathogenesis of schizophrenia, the relationship between FP volume and cognitive insight in this disorder is underexplored. We examined the relationship between cognitive insight and volume of FP using precise manual morphometry of high resolution magnetic resonance images in 19 schizophrenia patients (SCZ) and 21 healthy-volunteers (HV). The manual morphometry technique was replicated from a previous study based on a cytoarchitectonically and functionally valid definition of FP and cognitive insight was measured using Beck's cognitive insight scale. Left frontal pole volume was a significant predictor of self-reflection sub-score of Beck's cognitive insight scale (ß=0.68; t = 2.86; p = 0.01). A significant inverse relationship between age and bilateral FP volumes was noted in HV (left FP - r=-0.45; p = 0.04; right FP - r=-0.57; p = 0.008) but not in SCZ (p>0.05). Our findings provide anatomical substrates to devise intervention strategies targeting cognitive insight, thereby improving treatment adherence and functional outcomes.


Subject(s)
Schizophrenia , Cognition , Frontal Lobe/diagnostic imaging , Humans , Magnetic Resonance Imaging , Prefrontal Cortex/diagnostic imaging , Schizophrenia/diagnostic imaging
19.
J Phys Chem Lett ; 12(1): 302-309, 2021 Jan 14.
Article in English | MEDLINE | ID: mdl-33350833

ABSTRACT

Mn-doped perovskites have already been widely explored in the context of interesting optical, electronic, and magnetic properties. Such fascinating traits showcased by them explain the huge augmentation in the device efficiency, directing their widespread application in the field of solar cells, energy- harvesting sectors, and light-emitting diodes. However, the underlying photophysics governing the overall charge carrier dynamics in Mn-doped CsPbBr3 nanoplatelets (NPLs) has never been discussed and therefore demands an in-depth investigation. Herein, fluorescence up-conversion and femtosecond transient absorption (TA) spectroscopy are employed for gaining a comprehensive understanding of the excited-state dynamics and the fundamental energy/charge-transfer processes for two-dimensional CsPbBr3 nanoplatelets (NPLs) and their Mn-doped counterparts. The up-conversion measurement clearly suggests the possibility of energy-transfer pathways in the Mn-doped CsPbBr3 NPLs. Interestingly, strong indication of charge transfer (CT) in Mn-doped CsPbBr3 NPLs was unambiguously established by an ultrafast TA approach. Our investigation clearly suggests that both the probable processes viz. the ultrafast energy and electron transfers noticeable in the Mn2+-doped CsPbBr3 NPLs are utterly competitive and rapid owing to the highly confined nature of the two-dimensional NPLs. This extensive probing of concurrent charge/energy-transfer processes may pave help clarify unresolved anomalies in Mn-doped perovskites, which may prove advantageous for a wide range of practical applicability.

20.
J Phys Chem Lett ; 11(15): 6344-6352, 2020 Aug 06.
Article in English | MEDLINE | ID: mdl-32663017

ABSTRACT

The performance of the high-end optoelectronic devices is essentially influenced by the intrinsic relaxation mechanisms pursued by the hot carriers. Therefore, the key toward achieving progression in such fields lies in developing a complete understanding of the involved carrier cooling dynamics. In this work, an endeavor has been made to highlight the difference in the cooling mechanisms in 2D CsPbBr3 nanosheets (NSs) and their 3D counterpart nanocrystals (NCs) with the aid of femtosecond broad-band pump-probe spectroscopy, varying the excitation energies. The exciton and biexciton dynamics in both systems are found to be retarded upon increasing the excitation energy. However, in contrast to 3D NCs, carrier cooling is found to be faster in the 2D system, regardless of the excitation energy used, attributing this to less efficient charge screening by Fröhlich interaction in low-dielectric medium. A similar trend is replicated in the biexciton formation rate since the formation is also found to be faster in NSs compared to NCs.

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