Frequency and Temperature Effects on Trapped Centers Activation and Charge Transport Mechanism in Y0.2Ca0.8MnO3

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Shehzad, Matiullah Shah, Airfa Sakhawat, M. Nadeem, K. Mehmood, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7290143/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 21 Nov, 2025 Read the published version in Journal of Low Temperature Physics → Version 1 posted 12 You are reading this latest preprint version Abstract Perovskite type manganites Y 1 − x Ca xF MnO 3 in the composition range of x = 0.2 of orthorhombic crystal structure was synthesized through solid state route. Synchrotron XRD was cast-off for checking phase configuration using XRD and with support of freely available Fullprof program. Different structural parameters were measured after refinement of data. Impedance spectroscopy was useful to discover response of diverse electrical characteristics like conduction mechanism, electrical conductivity, different relaxation processes and capacitance of probed sample under the variation of temperature and frequency. Electrical constraints of grain boundaries specify a deviation in electrical transport phenomena about 110°K termed as T MI . Different electrical parameters were evaluated in terms of temperature and frequency effects on conduction mechanism through hopping having double exchange through Mn 3+ and Mn 4+ Manganites Impedance spectroscopy Conduction mechanism Conduction models Activation energy VRH SPH ARH Synchrotron XRD Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 Figure 10 Introduction Perovskite manganite materials (R 1 − x A x MnO 3 ) have been widely used in the field of research owing to their interesting electric and magnetic characters and they have drawn attention due to existence of certain contending propensities in their rich phase diagrams to entice large consideration with variety of orbital, spin, & charge ordering [ 1 – 3 ]. At first, this curiosity was sparked by detection of huge negative colossal magnetoresistance termed as CMR but far along many more thought-provoking features came into account [4–6]. Doped manganite materials in terms of complete phase competing properties of Y 1 − x Ca x MnO 3 is investigated with dependence on temperature, divalent concentration (x) and frequency through which we explored diversity of phases displayed in them which is character of manganites [7,8]. At x = 0 the material’s behavior is non-conducting and its resistivity is large, getting higher with lowering temperature. Initially it is paramagnetic but below curie temperature, it becomes anti ferro magnetic. For intermediate doping concentration 0.2 < x < 0.45 it exhibits metal-insulator (M-I) transition along strong FM to PM transition over a series of carrier concentrations and temperatures. As temperature is raised in this range there is a ferromagnetic-paramagnetic transition [9]. This shows that resistivity at T < T MI is relatively small and rises as temperature increases. These manganites show assembly of magnetic, electronic and structural phase transitions by varying temperature, composition, magnetic field, doping concentration and voltage. Initially these manganites exhibit antiferromagnetic behavior while by various perturbations like temperature, frequency and pressure, a change in phase can be seen [ 10 – 11 ]. In general manganese possesses and non-conducting nature, however with doping it starts playing an important role in conduction mechanism due to its double exchange mechanism having 3d orbital five-fold splitting. The doping level x = 0.2 exhibits strong metal to insulator transition. At low field effects in polycrystalline CMR compounds grains and grain boundaries show an imperative character. The polarons are closely related to electrical transport mechanism of doped manganites between their localized charged states [ 12 , 13 ]. The electric transport mechanism along with the electrical behavior of Y 0.2 Ca 0.8 MnO 3 is discussed in detailed using impedance spectroscopy. This is because it can independently measure real and imaginary part of complex electrical properties in range of applied frequencies and temperature resulting in a change in resistivity due to grains (Gs) and grain boundaries (Gbs). The co-existing electrical conduction and relaxation phenomena in this manganite, is probed for charged transport. In this text the magnetic, AC, electrical and structural behaviors are discussed. This family of manganites shows that antiferromagnetic and the ferromagnetic nature frequently presents itself at the same time over a series of temperatures [ 14 ]. Materials and Methods Solid-state reactions method was utilized to synthesize Y 0.2 Ca 0.8 MnO 3 by taking different precursor oxides (of Sigma Aldrich with 99.99% purity) like Y 2 O 3 , CaCO 3 and Mn 2 O 3 with stoichiometric molar amount [ 15 ]. These oxides and carbonates were mixed and grinded into fine powder. Heat treatments for 1000 o C, 1100 o C and 1200 o C for 16h of gradual increment of 5 o C/min with intermediate grinding were carried out. Then powder was ground and pellets of about (13mm diameter and 1.3mm thickness) were formed by applying hydraulic pressure of 3 ton/inch 2 . For the structural study of our sample, Bruker-D8 advanced diffractometer was employed with Cu-Kα as an x-ray source was used in which a mirror focused the incident beam vertically and made it monochromatic having a wavelength of 1.5406 Å. XRD measurements were recorded for the range of an angle 2θ from 10° to 90° with 0.0204 o of step size between two successive readings. Freely available FullProf program was incorporated for XRD data refinement [ 16 ]. Impedance spectroscopic method was applied in the frequency range 1Hz-10 7 Hz with temperature of about 78°K-298°K for electrical study[ 17 , 18 ]. Pallets were refined on each side to eradicate contamination and connected through silver paste. After being set aside in a homemade sample holder at room temperature for 1h the pellets were placed in Dewar of liquid Nitrogen for the examination of minor temperature effect by plummeting sample holder. Through D.C power supply temperature was made stable. Impedance analyzer (Novo control Alpha-N) controlled by WINDATA program running from pc was used by applying 0.5V A.C on the probed material. Regular measurements at a step size of 5K were taken. ZVIEW software with 2–3% fitting errors was employed for data attainment. Results Structural study was attained using synchrotron XRD for sample Y 0.2 Ca 0.8 MnO 3 . Through FullProf program x-ray spectrum as shown in Fig [1], was obtained in which red dot denotes the observed data, the measured data are shown by black lines, blue shows difference between observed and measured values and green bars signify Bragg’s position [19]. The space group Pbnm whose symmetry approves with composition of Y 0.2 Ca 0.8 MnO 3 shows single-phase structures characterized by the fitting of theoretical lines with observed data. Some lattice parameters of Y 0.2 Ca 0.8 MnO 3 are measured as: a = 5.47464Å b = 5.46834Å & c = 7.71621Å. This refinement is simulated for the reliability factor of χ 2 = 2.97. The χ 2 < 5 shows a good fitting [20]. Fig[2a] presents Nyquist plot at temperature of 78°K showing strong temperature dependence. At high frequency lower resistivity semicircles are attributed to Gs while at low frequency semicircles is qualified to GBs which acts as barrier to capture charge carriers due to defects and greater opposition is offered leading to semiconducting behavior [21]. Full spectrum of impedance plane plot Fig[2b] confirms that arcs of Nyquist plot raises with decrease of temperature. It concludes that resistance rises with decreasing temperature having lowest value for 298°K. The expansion in size of plot with temperature approves similar consequence shown in La 0.65 Ca 0.35 MnO 3 by M. Nadeem et al [22]. In the semicircle of Nyquist plot, a depression angle shows deviation of center from the x-axis. Fig [3] tells its variation with temperature and confirms that below room temperature the depression angle decreases emerging a clear well at 110°K. Between different phase results, the dynamic struggle from heterogenous environment of the ground state in these complexes, and the variations are improved nearby the grain boundary where two or more ordering contests [23]. Fig [4a] represents the loss spectrum which is used to investigate large resistive phase in the sample. Two prominent charms of this plot are location and intensity of peak. With rise in temperature peaks of spectrum condense to higher frequency region representing higher carrier mobility and reduce of relaxation time qualified to semiconducting behavior of the sample. It is also noteworthy that at higher frequency broaden shoulder like peaks with low intensity appear due to Gs however at trivial frequency side sharp peaks with high intensity occur due to GBs [23]. The enlargement of peak is owing to upsurge in thermal activation of dipoles. Frequency at peak points of spectrum is termed as relaxation frequency specified by f max =1/(2πτ) (τ = relaxation time). In Fig[4b] relaxation frequency of loss spectrum drawn against temperature transfer to advance frequency side by increasing temperature directing a lift in relaxation frequencies at Gs and GBs. A change in trend is observed around 110°K marked as metal insulator transition temperature T MI . With an increase in temperature there is a steady rise in relaxation frequency drawing the conclusion that electrons are thermally stimulated to hop through Mn 3+ and Mn 4+ responsible for conduction in Y 0.2 Ca 0.8 MnO 3 [24]. The frequency consequence on impedance’s real part Zʹ is revealed in Fig [5a] which shows two regions with increasing frequency as frequency dependent and independent region. Frequency independent portion grows with an upsurge in temperature, and also at low frequencies there is a drop in Zʹ which is due to the release of confined charge resulting in a rise in carrier motion. This at last initiates to converge at a single point due to discharge of all the space charges at higher frequency [25]. Fig [5b] represents the relaxation frequency obtained from the previous figure, and is plotted with temperature showing change in trend observed around 110°K above which there is decrease in relaxation frequency with rise in T. Electrical conductivity gives information about charge passage in Y 0.2 Ca 0.8 MnO 3 . Fig [6] exhibits conductivity with frequency dependence at diverse temperatures in which two regions can be observed. At a small frequency, frequency independent region correlates with D.C conductivity whereas the frequency dependent dispersion region is visible at higher frequency and with rise in temperature this dispersion region slowly reduces vanishing outside the given frequency range [26]. Fig [7] presents plot of capacitance versus temperature showing that the value of capacitance remains constant at initial temperature values because charge carriers do not get enough thermal energy to show any kind of mobility. However, when temperature reaches 110°K there is a boost in capacitance expressing exponential trend with increase in temperature which occurs due to grains [27]. Conduction mechanism of charge carriers is displayed in Fig [8] using SPH model in which resistance of said sample is plotted against temperature by an equation R/T = E o exp[E a /K b T]. By linear fitting on plot change in trend is observed around 110K ( T MI ). At temperatures higher than this, polarons jump from one lattice position to the next by thermal activation. When E a ≤200meV then conduction will be due to e − as in our case it is measured as 40.14 meV confirming that charge carriers are electrons [27]. By equivalent circuit model Arrhenius model is plotted in Fig [9] by expression R = R o exp(-E a /K b T). Conduction mechanism grows with lowering resistance signifying increase in mobility of charge carriers because GBs resistance contribution dominates over Gs. A small irregularity is observed around T MI =110°K where material behavior changes. Arrhenius Model is used to describe the kinetics of an activated process [28–29]. Fig. shows two slopes which intersect at 110°K and the values of these slopes are used to evaluate the activation energies E a which are measured as 44.11meV and 31.57meV at dissimilar frequencies [30]. These E a are of the same order as measured by SPH model. VRH model debates the conduction mechanism with localized charge carriers at low temperature, which is plotted in Fig[10a] using Mott expression [27,31] as R = R o exp(T o /T) 1/4 . T o is the temperature factor assumed by T o =18∝ 3 /K b N s (E F ) while N s (E F )\(\:=\:\)state density [18] and 1/∝=L is used to calculate the localization length [32–33]. Figure shows the charge transmission process marked for Y 0.2 Ca 0.8 MnO 3 at temperatures lower than 110°K during which polarons trip from one to another lattice position having a lower energy most probably to lengthier path [34]. VRH model [35–36] in terms of conductivity is expressed as σ = σ o exp[-B/T 0.25 ] where B = 4E a /(K b T 0.75 ). The σ versus T 0.25 for frequency of 4.71×10 5 Hz is plotted in Fig[10b] which shows that conductivity starts its increasing linear trend around 110°K and deviate above 110°K indicating a change in the conduction mechanism, declaring that the VRH model shows conduction in insulating region [37]. Conclusions Single phase and an orthorhombic Pbnm structure of synthesized Y 0.2 Ca 0.8 MnO 3 was found with employing XRD technique and electrical studies show the existence of metal-insulator change around 110K. Conduction mechanisms were studied through different conduction models. Different relaxation frequencies show thermal activation above 110K attributed to its metallic behavior at high temperature. Arrhenius model, SPH model and VRH models show a change in the conduction mechanism around 110k. At low temperature VRH model is followed and a higher value of resistance at low temperature indicates insulating behavior below 110K. Thermal activation energy of 40.14 is required to delocalize the charge carriers concluding that conduction in Y0.2Ca0.8MnO3 is due to the mobility of electrons. Declarations Author Contribution 1.K. Shehzad2. Matiullah Shah3. Airfa sakhawat4. M. Nadeem5. K. Mehmood 6. Saadat Khan 7. Q. Ain8. B. Maryam9. Anas Ramzan 10. Uzma Ghazanfar:Component of the researchAuthor’s numbeSubstantial contribution to conception and design1, 2, 4Substantial contribution to the acquisition of data 1, 3, 7, 8Substantial contribution to analysis and interpretation of data 2, 9, 10, Drafting the article5, 6Critically revising the article for important intellectual content2, 5, 10 Final approval of the version to be published1, 2, 3 Acknowledgements The authors acknowledge the experimental and lab support of PCG, Directorate of Science, PINSTech and HEC Pakistan. 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Cite Share Download PDF Status: Published Journal Publication published 21 Nov, 2025 Read the published version in Journal of Low Temperature Physics → Version 1 posted Editorial decision: Revision requested 11 Sep, 2025 Reviews received at journal 19 Aug, 2025 Reviews received at journal 14 Aug, 2025 Reviewers agreed at journal 07 Aug, 2025 Reviewers agreed at journal 05 Aug, 2025 Reviewers agreed at journal 05 Aug, 2025 Reviewers agreed at journal 04 Aug, 2025 Reviewers agreed at journal 04 Aug, 2025 Reviewers invited by journal 04 Aug, 2025 Editor assigned by journal 04 Aug, 2025 Submission checks completed at journal 04 Aug, 2025 First submitted to journal 04 Aug, 2025 You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Nadeem","email":"","orcid":"","institution":"PINSTECH Islamabad","correspondingAuthor":false,"prefix":"","firstName":"M.","middleName":"","lastName":"Nadeem","suffix":""},{"id":496111506,"identity":"70e4b5a3-7f4f-4d18-9bfb-ebf6e70732e4","order_by":4,"name":"K. Mehmood","email":"","orcid":"","institution":"Ghazi University","correspondingAuthor":false,"prefix":"","firstName":"K.","middleName":"","lastName":"Mehmood","suffix":""},{"id":496111507,"identity":"71acd045-3083-40b5-807c-979c7129e1fe","order_by":5,"name":"Saadat Khan","email":"","orcid":"","institution":"SUIT","correspondingAuthor":false,"prefix":"","firstName":"Saadat","middleName":"","lastName":"Khan","suffix":""},{"id":496111508,"identity":"df80e40c-2dcc-4e42-8fb0-16b6491987c6","order_by":6,"name":"Q. Ain","email":"","orcid":"","institution":"University of Wah","correspondingAuthor":false,"prefix":"","firstName":"Q.","middleName":"","lastName":"Ain","suffix":""},{"id":496111509,"identity":"5ebd2537-9357-4684-9dee-16adff97034d","order_by":7,"name":"B. Maryam","email":"","orcid":"","institution":"University of Wah","correspondingAuthor":false,"prefix":"","firstName":"B.","middleName":"","lastName":"Maryam","suffix":""},{"id":496111510,"identity":"ad75d7f2-a9ec-4042-8b3a-926043821996","order_by":8,"name":"Anas Ramzan","email":"","orcid":"","institution":"University of Wah","correspondingAuthor":false,"prefix":"","firstName":"Anas","middleName":"","lastName":"Ramzan","suffix":""},{"id":496111511,"identity":"4d7afc17-149d-4e1d-a2cc-3d05d5ca2ef3","order_by":9,"name":"Uzma Ghazanfar","email":"","orcid":"","institution":"University of Wah","correspondingAuthor":false,"prefix":"","firstName":"Uzma","middleName":"","lastName":"Ghazanfar","suffix":""}],"badges":[],"createdAt":"2025-08-04 10:38:35","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7290143/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7290143/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1007/s10909-025-03340-0","type":"published","date":"2025-11-21T15:58:37+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":88478089,"identity":"2a893de8-31f9-4752-9065-e164860fb229","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":83208,"visible":true,"origin":"","legend":"\u003cp\u003eRefined Synchrotron XRD pattern, red dots show observed data, black line shows calculated data and bars show Bragg’s positions.\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/513e6d82e7e71038f5043f89.png"},{"id":88478288,"identity":"b2a76773-d709-4325-8b85-2a71e32694a8","added_by":"auto","created_at":"2025-08-06 22:52:30","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":527780,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/277a8342fb201985a584618f.png"},{"id":88478091,"identity":"46504fd7-a83e-43de-9205-35d8d9857d8d","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":432925,"visible":true,"origin":"","legend":"\u003cp\u003eDepression angle of Nyquest plot semicircles plotted against temperature shows deviation of trend at 110K.\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/0330fbf44b8ecb5f0bcb3ddb.png"},{"id":88478094,"identity":"947c3d13-6d33-4f36-8063-8b75a6cb6f6c","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":871559,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/950b7567b279d562ff66de85.png"},{"id":88478290,"identity":"ea9380f3-f512-466d-ac6e-b843cfd0ced9","added_by":"auto","created_at":"2025-08-06 22:52:30","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":1056094,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/b5ce85d6b17696e6708e07a8.png"},{"id":88478773,"identity":"e9a5c3f8-ca6b-44c6-b200-f3b96e884bc5","added_by":"auto","created_at":"2025-08-06 23:08:30","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":425440,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/3e4e7bebd928f42689e2aedd.png"},{"id":88478296,"identity":"2c2bced7-164c-4eab-9be7-744497d4a74f","added_by":"auto","created_at":"2025-08-06 22:52:30","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":257620,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/d4f8fa1724c52be555d48eb0.png"},{"id":88478115,"identity":"9041eeef-e083-4a04-94b4-670b080edd97","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":418384,"visible":true,"origin":"","legend":"\u003cp\u003eTemperature dependence of resistance plotted according to SPH model.\u003c/p\u003e","description":"","filename":"8.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/9be9a8cd80a3ad442febb476.png"},{"id":88478101,"identity":"92bc4b03-c10d-461d-8736-da764017f697","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":256523,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"9.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/ea73008560e8c00947a969bb.png"},{"id":88478109,"identity":"e60ea70b-7480-4aa9-a363-db445cdf3d9a","added_by":"auto","created_at":"2025-08-06 22:44:30","extension":"png","order_by":10,"title":"Figure 10","display":"","copyAsset":false,"role":"figure","size":780185,"visible":true,"origin":"","legend":"\u003cp\u003eSee image above for figure legend\u003c/p\u003e","description":"","filename":"10.png","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/fbdc72b143c0cd31c7679b8d.png"},{"id":96651087,"identity":"7d9df98c-df10-49e0-be27-0895d4a08fb4","added_by":"auto","created_at":"2025-11-24 16:13:47","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":4314631,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7290143/v1/732a72ac-d80a-4ec3-b93b-3b60c497c61f.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"\u003cp\u003eFrequency and Temperature Effects on Trapped Centers Activation and Charge Transport Mechanism in Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e","fulltext":[{"header":"Introduction","content":"\u003cp\u003ePerovskite manganite materials (R\u003csub\u003e1\u0026thinsp;\u0026minus;\u0026thinsp;x\u003c/sub\u003eA\u003csub\u003ex\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e) have been widely used in the field of research owing to their interesting electric and magnetic characters and they have drawn attention due to existence of certain contending propensities in their rich phase diagrams to entice large consideration with variety of orbital, spin, \u0026amp; charge ordering [\u003cspan additionalcitationids=\"CR2\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. At first, this curiosity was sparked by detection of huge negative colossal magnetoresistance termed as CMR but far along many more thought-provoking features came into account [4\u0026ndash;6]. Doped manganite materials in terms of complete phase competing properties of Y\u003csub\u003e1\u0026thinsp;\u0026minus;\u0026thinsp;x\u003c/sub\u003eCa\u003csub\u003ex\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e is investigated with dependence on temperature, divalent concentration (x) and frequency through which we explored diversity of phases displayed in them which is character of manganites [7,8]. At x\u0026thinsp;=\u0026thinsp;0 the material\u0026rsquo;s behavior is non-conducting and its resistivity is large, getting higher with lowering temperature. Initially it is paramagnetic but below curie temperature, it becomes anti ferro magnetic. For intermediate doping concentration 0.2\u0026thinsp;\u0026lt;\u0026thinsp;x\u0026thinsp;\u0026lt;\u0026thinsp;0.45 it exhibits metal-insulator (M-I) transition along strong FM to PM transition over a series of carrier concentrations and temperatures. As temperature is raised in this range there is a ferromagnetic-paramagnetic transition [9]. This shows that resistivity at T\u0026thinsp;\u0026lt;\u0026thinsp;T\u003csub\u003eMI\u003c/sub\u003e is relatively small and rises as temperature increases. These manganites show assembly of magnetic, electronic and structural phase transitions by varying temperature, composition, magnetic field, doping concentration and voltage. Initially these manganites exhibit antiferromagnetic behavior while by various perturbations like temperature, frequency and pressure, a change in phase can be seen [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e10\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e11\u003c/span\u003e]. In general manganese possesses and non-conducting nature, however with doping it starts playing an important role in conduction mechanism due to its double exchange mechanism having 3d orbital five-fold splitting. The doping level x\u0026thinsp;=\u0026thinsp;0.2 exhibits strong metal to insulator transition. At low field effects in polycrystalline CMR compounds grains and grain boundaries show an imperative character. The polarons are closely related to electrical transport mechanism of doped manganites between their localized charged states [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e12\u003c/span\u003e, \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. The electric transport mechanism along with the electrical behavior of Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e is discussed in detailed using impedance spectroscopy. This is because it can independently measure real and imaginary part of complex electrical properties in range of applied frequencies and temperature resulting in a change in resistivity due to grains (Gs) and grain boundaries (Gbs). The co-existing electrical conduction and relaxation phenomena in this manganite, is probed for charged transport. In this text the magnetic, AC, electrical and structural behaviors are discussed. This family of manganites shows that antiferromagnetic and the ferromagnetic nature frequently presents itself at the same time over a series of temperatures [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e14\u003c/span\u003e].\u003c/p\u003e"},{"header":"Materials and Methods","content":"\u003cp\u003eSolid-state reactions method was utilized to synthesize Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e by taking different precursor oxides (of Sigma Aldrich with 99.99% purity) like Y\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e, CaCO\u003csub\u003e3\u003c/sub\u003e and Mn\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e with stoichiometric molar amount [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e15\u003c/span\u003e]. These oxides and carbonates were mixed and grinded into fine powder. Heat treatments for 1000\u003csup\u003eo\u003c/sup\u003eC, 1100\u003csup\u003eo\u003c/sup\u003eC and 1200\u003csup\u003eo\u003c/sup\u003eC for 16h of gradual increment of 5\u003csup\u003eo\u003c/sup\u003eC/min with intermediate grinding were carried out. Then powder was ground and pellets of about (13mm diameter and 1.3mm thickness) were formed by applying hydraulic pressure of 3 ton/inch\u003csup\u003e2\u003c/sup\u003e. For the structural study of our sample, Bruker-D8 advanced diffractometer was employed with Cu-Kα as an x-ray source was used in which a mirror focused the incident beam vertically and made it monochromatic having a wavelength of 1.5406 \u0026Aring;. XRD measurements were recorded for the range of an angle 2θ from 10\u0026deg; to 90\u0026deg; with 0.0204\u003csup\u003eo\u003c/sup\u003e of step size between two successive readings. Freely available FullProf program was incorporated for XRD data refinement [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e16\u003c/span\u003e]. Impedance spectroscopic method was applied in the frequency range 1Hz-10\u003csup\u003e7\u003c/sup\u003eHz with temperature of about 78\u0026deg;K-298\u0026deg;K for electrical study[\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e17\u003c/span\u003e, \u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e18\u003c/span\u003e]. Pallets were refined on each side to eradicate contamination and connected through silver paste. After being set aside in a homemade sample holder at room temperature for 1h the pellets were placed in Dewar of liquid Nitrogen for the examination of minor temperature effect by plummeting sample holder. Through D.C power supply temperature was made stable. Impedance analyzer (Novo control Alpha-N) controlled by WINDATA program running from pc was used by applying 0.5V A.C on the probed material. Regular measurements at a step size of 5K were taken. ZVIEW software with 2\u0026ndash;3% fitting errors was employed for data attainment.\u003c/p\u003e"},{"header":"Results","content":"\u003cp\u003eStructural study was attained using synchrotron XRD for sample Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e. Through FullProf program x-ray spectrum as shown in Fig [1], was obtained in which red dot denotes the observed data, the measured data are shown by black lines, blue shows difference between observed and measured values and green bars signify Bragg’s position [19]. The space group \u003cem\u003ePbnm\u003c/em\u003e whose symmetry approves with composition of Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e shows single-phase structures characterized by the fitting of theoretical lines with observed data. Some lattice parameters of Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e are measured as: a = 5.47464Å b = 5.46834Å \u0026amp; c = 7.71621Å. This refinement is simulated for the reliability factor of χ\u003csup\u003e2\u003c/sup\u003e = 2.97. The χ\u003csup\u003e2\u003c/sup\u003e \u0026lt; 5 shows a good fitting [20].\u003c/p\u003e\n\u003cp\u003eFig[2a] presents Nyquist plot at temperature of 78°K showing strong temperature dependence. At high frequency lower resistivity semicircles are attributed to Gs while at low frequency semicircles is qualified to GBs which acts as barrier to capture charge carriers due to defects and greater opposition is offered leading to semiconducting behavior [21].\u003c/p\u003e\n\u003cp\u003eFull spectrum of impedance plane plot Fig[2b] confirms that arcs of Nyquist plot raises with decrease of temperature. It concludes that resistance rises with decreasing temperature having lowest value for 298°K. The expansion in size of plot with temperature approves similar consequence shown in La\u003csub\u003e0.65\u003c/sub\u003eCa\u003csub\u003e0.35\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e by M. Nadeem et al [22].\u003c/p\u003e\n\u003cp\u003eIn the semicircle of Nyquist plot, a depression angle shows deviation of center from the x-axis. Fig [3] tells its variation with temperature and confirms that below room temperature the depression angle decreases emerging a clear well at 110°K. Between different phase results, the dynamic struggle from heterogenous environment of the ground state in these complexes, and the variations are improved nearby the grain boundary where two or more ordering contests [23].\u003c/p\u003e\n\u003cp\u003eFig [4a] represents the loss spectrum which is used to investigate large resistive phase in the sample. Two prominent charms of this plot are location and intensity of peak. With rise in temperature peaks of spectrum condense to higher frequency region representing higher carrier mobility and reduce of relaxation time qualified to semiconducting behavior of the sample. It is also noteworthy that at higher frequency broaden shoulder like peaks with low intensity appear due to Gs however at trivial frequency side sharp peaks with high intensity occur due to GBs [23]. The enlargement of peak is owing to upsurge in thermal activation of dipoles.\u003c/p\u003e\n\u003cp\u003eFrequency at peak points of spectrum is termed as relaxation frequency specified by f\u003csub\u003emax\u003c/sub\u003e=1/(2πτ) (τ = relaxation time). In Fig[4b] relaxation frequency of loss spectrum drawn against temperature transfer to advance frequency side by increasing temperature directing a lift in relaxation frequencies at Gs and GBs. A change in trend is observed around 110°K marked as metal insulator transition temperature T\u003csub\u003eMI\u003c/sub\u003e. With an increase in temperature there is a steady rise in relaxation frequency drawing the conclusion that electrons are thermally stimulated to hop through Mn\u003csup\u003e3+\u003c/sup\u003e and Mn\u003csup\u003e4+\u003c/sup\u003e responsible for conduction in Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e [24].\u003c/p\u003e\n\u003cp\u003eThe frequency consequence on impedance’s real part Zʹ is revealed in Fig [5a] which shows two regions with increasing frequency as frequency dependent and independent region. Frequency independent portion grows with an upsurge in temperature, and also at low frequencies there is a drop in Zʹ which is due to the release of confined charge resulting in a rise in carrier motion. This at last initiates to converge at a single point due to discharge of all the space charges at higher frequency [25].\u003c/p\u003e\n\u003cp\u003eFig [5b] represents the relaxation frequency obtained from the previous figure, and is plotted with temperature showing change in trend observed around 110°K above which there is decrease in relaxation frequency with rise in T.\u003c/p\u003e\n\u003cp\u003eElectrical conductivity gives information about charge passage in Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e. Fig [6] exhibits conductivity with frequency dependence at diverse temperatures in which two regions can be observed. At a small frequency, frequency independent region correlates with D.C conductivity whereas the frequency dependent dispersion region is visible at higher frequency and with rise in temperature this dispersion region slowly reduces vanishing outside the given frequency range [26].\u003c/p\u003e\n\u003cp\u003eFig [7] presents plot of capacitance versus temperature showing that the value of capacitance remains constant at initial temperature values because charge carriers do not get enough thermal energy to show any kind of mobility. However, when temperature reaches 110°K there is a boost in capacitance expressing exponential trend with increase in temperature which occurs due to grains [27].\u003c/p\u003e\n\u003cp\u003eConduction mechanism of charge carriers is displayed in Fig [8] using SPH model in which resistance of said sample is plotted against temperature by an equation R/T = E\u003csub\u003eo\u003c/sub\u003eexp[E\u003csub\u003ea\u003c/sub\u003e/K\u003csub\u003eb\u003c/sub\u003eT]. By linear fitting on plot change in trend is observed around 110K (\u003cstrong\u003eT\u003c/strong\u003e\u003csub\u003e\u003cstrong\u003eMI\u003c/strong\u003e\u003c/sub\u003e). At temperatures higher than this, polarons jump from one lattice position to the next by thermal activation. When E\u003csub\u003ea\u003c/sub\u003e≤200meV then conduction will be due to e\u003csup\u003e−\u003c/sup\u003e as in our case it is measured as 40.14 meV confirming that charge carriers are electrons [27].\u003c/p\u003e\n\u003cp\u003eBy equivalent circuit model Arrhenius model is plotted in Fig [9] by expression R = R\u003csub\u003eo\u003c/sub\u003eexp(-E\u003csub\u003ea\u003c/sub\u003e/K\u003csub\u003eb\u003c/sub\u003eT). Conduction mechanism grows with lowering resistance signifying increase in mobility of charge carriers because GBs resistance contribution dominates over Gs. A small irregularity is observed around T\u003csub\u003eMI\u003c/sub\u003e=110°K where material behavior changes. Arrhenius Model is used to describe the kinetics of an activated process [28–29]. Fig. shows two slopes which intersect at 110°K and the values of these slopes are used to evaluate the activation energies E\u003csub\u003ea\u003c/sub\u003e which are measured as 44.11meV and 31.57meV at dissimilar frequencies [30]. These E\u003csub\u003ea\u003c/sub\u003e are of the same order as measured by SPH model.\u003c/p\u003e\n\u003cp\u003eVRH model debates the conduction mechanism with localized charge carriers at low temperature, which is plotted in Fig[10a] using Mott expression [27,31] as R = R\u003csub\u003eo\u003c/sub\u003eexp(T\u003csub\u003eo\u003c/sub\u003e/T)\u003csup\u003e1/4\u003c/sup\u003e. T\u003csub\u003eo\u003c/sub\u003e is the temperature factor assumed by T\u003csub\u003eo\u003c/sub\u003e=18∝\u003csup\u003e3\u003c/sup\u003e/K\u003csub\u003eb\u003c/sub\u003eN\u003csub\u003es\u003c/sub\u003e(E\u003csub\u003eF\u003c/sub\u003e) while N\u003csub\u003es\u003c/sub\u003e(E\u003csub\u003eF\u003c/sub\u003e)\\(\\:=\\:\\)state density [18] and 1/∝=L is used to calculate the localization length [32–33]. Figure shows the charge transmission process marked for Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e at temperatures lower than 110°K during which polarons trip from one to another lattice position having a lower energy most probably to lengthier path [34].\u003c/p\u003e\n\u003cp\u003eVRH model [35–36] in terms of conductivity is expressed as σ = σ\u003csub\u003eo\u003c/sub\u003e exp[-B/T\u003csup\u003e0.25\u003c/sup\u003e] where B = 4E\u003csub\u003ea\u003c/sub\u003e/(K\u003csub\u003eb\u003c/sub\u003eT\u003csup\u003e0.75\u003c/sup\u003e). The σ versus T \u003csup\u003e0.25\u003c/sup\u003e for frequency of 4.71×10\u003csup\u003e5\u003c/sup\u003eHz is plotted in Fig[10b] which shows that conductivity starts its increasing linear trend around 110°K and deviate above 110°K indicating a change in the conduction mechanism, declaring that the VRH model shows conduction in insulating region [37].\u003c/p\u003e"},{"header":"Conclusions","content":"\u003cp\u003eSingle phase and an orthorhombic \u003cem\u003ePbnm\u003c/em\u003e structure of synthesized Y\u003csub\u003e0.2\u003c/sub\u003eCa\u003csub\u003e0.8\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e was found with employing XRD technique and electrical studies show the existence of metal-insulator change around 110K. Conduction mechanisms were studied through different conduction models. Different relaxation frequencies show thermal activation above 110K attributed to its metallic behavior at high temperature. Arrhenius model, SPH model and VRH models show a change in the conduction mechanism around 110k. At low temperature VRH model is followed and a higher value of resistance at low temperature indicates insulating behavior below 110K. Thermal activation energy of 40.14 is required to delocalize the charge carriers concluding that conduction in Y0.2Ca0.8MnO3 is due to the mobility of electrons.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003e1.K. Shehzad2. Matiullah Shah3. Airfa sakhawat4. M. Nadeem5. K. Mehmood 6. Saadat Khan 7. Q. Ain8. B. Maryam9. Anas Ramzan 10. Uzma Ghazanfar:Component of the researchAuthor\u0026rsquo;s numbeSubstantial contribution to conception and design1, 2, 4Substantial contribution to the acquisition of data 1, 3, 7, 8Substantial contribution to analysis and interpretation of data 2, 9, 10, Drafting the article5, 6Critically revising the article for important intellectual content2, 5, 10 Final approval of the version to be published1, 2, 3\u003c/p\u003e\u003cp\u003e\u003cstrong\u003eAcknowledgements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u0026nbsp; \u0026nbsp;The authors acknowledge the experimental and lab support of PCG, Directorate of Science, PINSTech and HEC Pakistan.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eElbio Dagotto, Nanoscale Phase Separation and Colossal Magnetoresistance: The Physics of Manganites and Related Compounds, Springer Series, New York, 2003.\u003c/li\u003e\n\u003cli\u003eY.Moualhi, H.Rahmouni, K.Khirouni, Usefulness of theoretical approaches and experiential conductivity measurements for understanding manganite-transport mechanisms, J. 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Mater. 519 (2021) 167450, https://doi.org/10.1016/j.jmmm.2020.167450. \u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"journal-of-low-temperature-physics","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"jltp","sideBox":"Learn more about [Journal of Low Temperature Physics](http://link.springer.com/journal/10909)","snPcode":"10909","submissionUrl":"https://submission.nature.com/new-submission/10909/3","title":"Journal of Low Temperature Physics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"Manganites, Impedance spectroscopy, Conduction mechanism, Conduction models, Activation energy, VRH, SPH, ARH, Synchrotron XRD","lastPublishedDoi":"10.21203/rs.3.rs-7290143/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7290143/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003ePerovskite type manganites Y\u003csub\u003e1\u0026thinsp;\u0026minus;\u0026thinsp;x\u003c/sub\u003eCa\u003csub\u003exF\u003c/sub\u003eMnO\u003csub\u003e3\u003c/sub\u003e in the composition range of x\u0026thinsp;=\u0026thinsp;0.2 of orthorhombic crystal structure was synthesized through solid state route. Synchrotron XRD was cast-off for checking phase configuration using XRD and with support of freely available Fullprof program. Different structural parameters were measured after refinement of data. Impedance spectroscopy was useful to discover response of diverse electrical characteristics like conduction mechanism, electrical conductivity, different relaxation processes and capacitance of probed sample under the variation of temperature and frequency. Electrical constraints of grain boundaries specify a deviation in electrical transport phenomena about 110\u0026deg;K termed as T\u003csub\u003eMI\u003c/sub\u003e. Different electrical parameters were evaluated in terms of temperature and frequency effects on conduction mechanism through hopping having double exchange through Mn\u003csup\u003e3+\u003c/sup\u003e and Mn\u003csup\u003e4+\u003c/sup\u003e\u003c/p\u003e","manuscriptTitle":"Frequency and Temperature Effects on Trapped Centers Activation and Charge Transport Mechanism in Y0.2Ca0.8MnO3","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-08-06 22:44:25","doi":"10.21203/rs.3.rs-7290143/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2025-09-11T19:21:56+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-08-19T09:52:56+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2025-08-14T10:55:06+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"319990694889249637130317635804111411711","date":"2025-08-08T03:22:39+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"305616873141210927143625469452361616526","date":"2025-08-05T15:17:37+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"256850749702878025695130506292139274978","date":"2025-08-05T06:49:49+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"79233058530456244724608881216221751363","date":"2025-08-05T03:07:08+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"191102029027129015328204117110615857729","date":"2025-08-04T19:47:47+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2025-08-04T16:16:22+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2025-08-04T14:22:32+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2025-08-04T14:21:51+00:00","index":"","fulltext":""},{"type":"submitted","content":"Journal of Low Temperature Physics","date":"2025-08-04T10:37:03+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"journal-of-low-temperature-physics","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"jltp","sideBox":"Learn more about [Journal of Low Temperature Physics](http://link.springer.com/journal/10909)","snPcode":"10909","submissionUrl":"https://submission.nature.com/new-submission/10909/3","title":"Journal of Low Temperature Physics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"42a44d96-39fd-4ed1-bc88-5403b5f27ba6","owner":[],"postedDate":"August 6th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[],"tags":[],"updatedAt":"2025-11-24T16:11:48+00:00","versionOfRecord":{"articleIdentity":"rs-7290143","link":"https://doi.org/10.1007/s10909-025-03340-0","journal":{"identity":"journal-of-low-temperature-physics","isVorOnly":false,"title":"Journal of Low Temperature Physics"},"publishedOn":"2025-11-21 15:58:37","publishedOnDateReadable":"November 21st, 2025"},"versionCreatedAt":"2025-08-06 22:44:25","video":"","vorDoi":"10.1007/s10909-025-03340-0","vorDoiUrl":"https://doi.org/10.1007/s10909-025-03340-0","workflowStages":[]},"version":"v1","identity":"rs-7290143","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7290143","identity":"rs-7290143","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}