Self-Trapped-Exciton Radiative Recombination in β-Ga2O3: Impact of Two Concurrent Nonradiative Auger Processes.

IF 4.7 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC ACS Applied Electronic Materials Pub Date : 2025-02-17 eCollection Date: 2025-03-11 DOI:10.1021/acsaelm.4c02099
Vytautas Grivickas, Patrik Ščajev, Saulius Miasojedovas, Lars Voss, Paulius Grivickas
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Abstract

The peculiarities of radiative and nonradiative processes associated with self-trapped intrinsic eXcitons in the excited β-Ga2O3 crystals are studied via time-resolved techniques of induced absorption, transient grating, and photoluminescence (PL) at room temperature. The excitation above the bandgap is produced by laser pulses with linear light polarization parallel and orthogonal in the (-201) and (001) planes. We elucidate that the nonradiative recombination rate occurring in the eXciton prevails over its radiative emission rate in a wide range of free carrier concentration composed of excited and equilibrium electrons. Hence, the nonradiative recombination has no effect on the strong anisotropy and the shape of the eXciton emission band. However, we find out that the conventional ABC model of electron effective lifetime is insufficient for explanation of the excitation dependences. Inclusion of two nonradiative Auger mechanisms in a modified ABC formula provides excellent agreement of these dependences. We conclude that the trap-assisted Auger process is in proportion to the free electron density with coefficient B = 1.1 × 10-11 cm3/s and appears at low/intermediate excitation, while the triple-particle Auger process is in proportion to Δn 2 with coefficient C = 8 × 10-30 cm6/s and appears at high excitation conditions. The transition between two Auger mechanisms is accompanied by a rise of the eXciton diffusivity in preferred crystallographic directions where the radiative PL intensity is maximal. The diffusion length L D in these directions can reach values ∼300 nm, but, at high excitations, L D becomes limited by Auger lifetimes. These findings pave the way for the implementation of self-trapped eXcitons into specific optoelectronic devices.

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β-Ga2O3中自困激子辐射复合:两个同步非辐射俄歇过程的影响。
利用诱导吸收、瞬态光栅和室温光致发光等时间分辨技术,研究了受激β-Ga2O3晶体中与自捕获本征激子相关的辐射和非辐射过程的特性。在(-201)和(001)平面上平行和正交的线性光偏振激光脉冲产生带隙以上的激发。在由激发态和平衡态电子组成的自由载流子浓度范围内,激子的非辐射复合率高于其辐射发射率。因此,非辐射复合对强各向异性和激子发射带的形状没有影响。然而,我们发现传统的电子有效寿命的ABC模型不足以解释激发依赖性。在修改的ABC公式中包含两个非辐射俄歇机制,提供了这些依赖关系的极好一致性。综上所述,陷阱辅助俄歇过程与自由电子密度成正比,系数B = 1.1 × 10-11 cm3/s,出现在低/中激发条件下;三粒子俄歇过程与Δn 2成正比,系数C = 8 × 10-30 cm3/s,出现在高激发条件下。两种俄歇机制之间的转变伴随着激子扩散率在辐射PL强度最大的首选晶体方向上的上升。在这些方向上的扩散长度L D可以达到~ 300 nm,但是,在高激发下,L D受到俄歇寿命的限制。这些发现为在特定光电器件中实现自捕获激子铺平了道路。
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来源期刊
CiteScore
7.20
自引率
4.30%
发文量
567
期刊介绍: ACS Applied Electronic Materials is an interdisciplinary journal publishing original research covering all aspects of electronic materials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials science, engineering, optics, physics, and chemistry into important applications of electronic materials. Sample research topics that span the journal's scope are inorganic, organic, ionic and polymeric materials with properties that include conducting, semiconducting, superconducting, insulating, dielectric, magnetic, optoelectronic, piezoelectric, ferroelectric and thermoelectric. Indexed/​Abstracted: Web of Science SCIE Scopus CAS INSPEC Portico
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