Correlating the low-temperature photoluminescence with electron transport properties in cerium oxide thin film.

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL Journal of Chemical Physics Pub Date : 2025-02-07 DOI:10.1063/5.0244962
Mousri Paul, Sabyasachi Karmakar, Jay Sharma, Satyaban Bhunia, Supratic Chakraborty
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Abstract

The complex interaction between the intrinsic and extrinsic state variables of strongly correlated insulator thin films is drawing interest as it shows memristive behavior that may be applicable to neuromorphic computing. Cerium oxide is an interesting material as its band structure is modified due to the formation of oxygen vacancy defects. The polaron formation that results from the reduction of the Ce4+ state to the Ce3+ state through oxygen vacancies is crucial for the electron transport in cerium oxide and is strongly influenced by temperature. In this work, we examined the relationship between the change in band structure and the associated conductivity at lower temperatures when ceria is exposed to light. Following light excitation, the creation of oxygen vacancies results in electron localization in the Ce 4f state, followed by the electron transition from 4f1 to 4f0, generating the PL spectra. With decreasing temperature, the lattice vibration decreases, and the splitting in the PL peak at a particular energy state validates the weaker electron-phonon interaction with an exciton trap. This reduces the carrier mobility of the film as observed from the resistance vs temperature curve of ceria under dark conditions. When excited by a particular energy of light, the electrons move more easily from the defect state to the conduction band, increasing conductivity at much lower temperatures than the conductivity under dark conditions.

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氧化铈薄膜中低温光致发光与电子输运性质的关系。
强相关绝缘体薄膜的内在和外在状态变量之间的复杂相互作用引起了人们的兴趣,因为它显示出可能适用于神经形态计算的记忆行为。氧化铈是一种有趣的材料,它的能带结构由于氧空位缺陷的形成而被改变。由Ce4+态通过氧空位还原为Ce3+态导致的极化子形成对氧化铈中的电子传递至关重要,并且受温度的强烈影响。在这项工作中,我们研究了在较低温度下,当二氧化铈暴露于光中时,带结构的变化与相关电导率之间的关系。在光激发下,氧空位的产生导致电子定位在Ce 4f态,随后电子从4f1跃迁到4f0,产生PL光谱。随着温度的降低,晶格振动减小,并且在特定能量状态下PL峰的分裂验证了与激子阱的电子-声子相互作用较弱。这降低了薄膜的载流子迁移率,从黑暗条件下二氧化铈的电阻与温度曲线观察到。当被特定能量的光激发时,电子更容易从缺陷态移动到导带,在较低温度下的导电性比在黑暗条件下的导电性高得多。
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来源期刊
Journal of Chemical Physics
Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
7.40
自引率
15.90%
发文量
1615
审稿时长
2 months
期刊介绍: The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.
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