Broadband ultrafast photogenerated carrier dynamics induced by intrinsic defects in <inline-formula><tex-math id="Z-20231102113631">\begin{document}$\boldsymbol\beta$\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="21-20231173_Z-20231102113631.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="21-20231173_Z-20231102113631.png"/></alternatives></inline-formula>-Ga<sub>2</sub>O<sub>3</sub>

Wang Lu-Xuan; Liu Yi-Tong; Shi Fang-Yuan; Qi Xian-Wen; Shen Han; Song Ying-Lin; Fang Yu

doi:10.7498/aps.72.20231173

Abstract

The ultra-wide bandgap semiconductor gallium oxide β-Ga₂O₃ with enhanced resistance to the irradiation and temperature is favorable for high-power and high-temperature optoelectronic devices. β-Ga₂O₃ also exhibits great potential applications in the field of integrated photonics because of its compatibility with the CMOS technique. However, a variety of intrinsic and extrinsic defects and trap states coexist in β-Ga₂O₃, including vacancies, interstitials, and impurity atoms. The defect-related carrier dynamics in β-Ga₂O₃ not only adversely affect the optical and electrical properties, but also directly limit the performance of β-Ga₂O₃ based devices. Therefore, a comprehensive understanding of the carrier transportation and relaxation dynamics induced by intrinsic defects is very important. Supercontinuum-probe spectroscopy can provide a fruitful information about the carrier relaxation processes in different recombination mechanisms, and thus becomes an effective way to study the defect dynamics. In this work, we study the dynamics of carrier trapping and recombination induced by intrinsic defects in pristine β-Ga₂O₃ crystal by using wavelength-tunable ultrafast transient absorption spectroscopy. The broadband absorption spectra induced by the intrinsic defects are strongly dependent on the polarization of pump pulse and probe pulse. Particularly, two absorption peaks induced by the two defect states can be extracted from the transient absorption spectra by subtracting the absorption transients under two probe polarizations. The observed defect-induced absorption features are attributed to the optical transitions from the valence band to the different charge states of the intrinsic defects (such as gallium vacancy). The data are well explained by a proposed carrier capture model based on multi-level energies. Moreover, the hole capture rate is found to be much greater than that of the electron, and the absorption cross-section of the defect state is at least 10 times larger than that of free carrier. Our findings not only clarify the relationship between intrinsic defects and photogenerated carrier dynamics, but also show the importance in the application of β-Ga₂O₃ crystals in ultrafast and broadband photonics.

Keywords:

Authors and contacts

1.
Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application, School of Physical Science and Technology, Suzhou University of Science and Technology, Suzhou 215009, China
2.
School of Physical Science and Technology, Soochow University, Suzhou 215006, China

Corresponding author: Fang Yu, yufang@usts.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11704273), the Natural Science Foundation of Jiangsu Province, China (Grant No. BK20221384), the Jiangsu Key Disciplines of the Fourteenth Five-Year Plan, China (Grant No. 2021135), the Postgraduate Research & Practice Innovation Program of Jiangsu Province, China (Grant No. KYCX22_3267), and the Undergraduate Training Programs for Innovation and Entrepreneurship of Suzhou University of Science and Technology, China (Grant Nos. 202310332270X, 2022011002X).

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References

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[2]	Higashiwaki M, Kaplar R, Pernot J, Zhao H P 2021 Appl. Phys. Lett. 118 200401 Google Scholar
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[13]	Sun Y F, Li Z G, Fang Y, Wu X Z, Zhou W F, Jia Z T, Yang J Y, Song Y L 2022 Appl. Phys. Lett. 120 032101 Google Scholar
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[22]	Singh A, Koksal O, Tanen N, McCandless J, Jena D, Xing H G, Peelaers H, Rana F 2021 Phys. Rev. Res. 3 023154 Google Scholar
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[32]	Luchechko A, Vasyltsiv V, Zhydachevskyy Y, et al. 2020 J. Phys. D: Appl. Phys. 53 354001 Google Scholar
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[35]	Varley J B, Peelaers H, Janotti A, Van de Walle C G 2011 J. Phys. Condens. Matter 23 334212 Google Scholar
[36]	Deák P, Ho Q D, Seemann F, Aradi B, Lorke M, Frauenheim T 2017 Phys. Rev. B 95 075208 Google Scholar
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[41]	Zimmermann C, Rønning V, Frodason Y K, Bobal V, Vines L, Varley J B 2020 Phys. Rev. Mater. 4 074605 Google Scholar
[42]	Fang Y, Wu X Z, Yang J Y, Xiao Z G, Yang Y, Zhou F, Song Y L 2015 Appl. Phys. Lett. 107 051901 Google Scholar
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图 1 (a) UID和Sn掺杂β-Ga₂O₃的透射光谱, 箭头表示泵浦光波长; (b)不同入射光强下β-Ga₂O₃的开孔Z扫描曲线, 实线为理论拟合曲线

Figure 1. (a) Optical transmission spectra of UID and Sn-doped β-Ga₂O₃, where the arrow denotes the pump wavelength; (b) open-aperture Z-scan data of β-Ga₂O₃ at different incident light intensities, where the solid lines are theoretical fitting curves.

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图 2 在不同的延迟时间下, 沿(a) [010]和(b) [102]晶轴探测下UID β-Ga₂O₃晶体的瞬态吸收光谱; 沿(c) [010]和(d) [102]轴探测下提取的不同波长吸收衰减动力学. 泵浦脉冲固定为沿[102]轴偏振

Figure 2. Transient absorption spectra of the UID β-Ga₂O₃ crystal probed at different delay times for different probe polarizations with respect to the (a) [010] and (b) [102] crystal axes. Extracted decay dynamics of absorption under different probe wavelengths for probe polarization along the (c) [010] and (d) [102] axes. The pump pulse is fixed to be polarized along the [102] axis.

DownLoad: Full-Size Img PowerPoint

图 3 在t_d = 2 ps处沿(a) [010]和(b) [102]晶轴探测偏振下的缺陷吸收光谱(数据点); (c)两个探测偏振方向的差分瞬态吸收ΔmOD^*. 所有的缺陷吸收光谱都可以用两个高斯函数(虚线)进行拟合

Figure 3. Defect absorption spectra (dots) as a function of probe photon energy for polarization along the (a) [010] and (b) [102] crystal axes at t_d = 2 ps; (c) the difference transients ΔmOD^* between two probe polarization directions. All the defect absorption spectra can be fitted using two Gaussian functions (dashed lines).

DownLoad: Full-Size Img PowerPoint

图 4 双光子激发(2PE)载流子俘获和本征缺陷吸收图, V_Ga相关缺陷的多电荷态($ {2{\rm{V}}}_{{\rm{G}}{\rm{a}}}^{1}{\text{-}}{{\rm{G}}{\rm{a}}}_{{\rm{i}}}^{{\rm{c}}} $)可以被泵浦脉冲激发并允许载流子俘获和光学跃迁(探测脉冲所经历的瞬态吸收)

Figure 4. Diagram of two-photon excited (2PE) carrier capture and the intrinsic defect absorption, the multiple charge states of the V_Ga-related defects ($ {2{\rm{V}}}_{{\rm{G}}{\rm{a}}}^{1}{\text{-}}{{\rm{G}}{\rm{a}}}_{{\rm{i}}}^{{\rm{c}}} $ is for consideration) can be excited by pump pulses and allow carrier trapping (black arrows) and optical transitions (transient absorption experienced by the probe pulses).

DownLoad: Full-Size Img PowerPoint

图 5 (a)—(c)泵浦光沿[102]轴偏振时, 测量和拟合得到的不同探测偏振和波长下UID β-Ga₂O₃的吸收动力学

Figure 5. (a)–(c) Measured and computed absorption kinetics in UID β-Ga₂O₃ for different probe polarizations and wavelengths when pumped along the [102] axis.

DownLoad: Full-Size Img PowerPoint

表 1 提取的瞬态吸收动力学模型参数

Table 1. Extracted parameters to model the transient absorption kinetics.

参数	数值
N_d/cm³	(1.7±0.2)×10¹⁶
$C_{\text{p}}^{ - 2}$/(cm³·s)	(1.6±0.3)×10^–6
$C_{\text{p}}^{ - 1}$/(cm³·s)	(1.3±0.2)×10^–6
σ_{–1 \|max}// [010]/cm²	(1.4±0.4)×10^–17
σ_{–1 \|max}// [102]/cm²	(2.3±0.5)×10^–17
σ_{0 \|max}// [102]/cm²	(2.2±0.6)×10^–17

DownLoad: CSV

map

[1]	Pearton S J, Yang J C, Cary P H, Ren F, Kim J, Tadjer M J, Mastro M A 2018 Appl. Phys. Rev. 5 011301 Google Scholar
[2]	Higashiwaki M, Kaplar R, Pernot J, Zhao H P 2021 Appl. Phys. Lett. 118 200401 Google Scholar
[3]	Higashiwaki M, Sasaki K, Kuramata A, Masui T, Yamakoshi S 2012 Appl. Phys. Lett. 100 013504 Google Scholar
[4]	Chen X H, Ren F F, Gu S L, Ye 2019 Photonics Res. 7 381 Google Scholar
[5]	Guo D Y, Guo Q, Chen Z, Wu Z, Li P, Tang W H 2019 Mater. Today Phys. 11 100157 Google Scholar
[6]	Tadjer M J, Lyons J L, Nepal N, Freitas Jr J A, Koehler A D, Foster G M 2019 ECS J. Solid State Sci. Technol. 8 Q3187 Google Scholar
[7]	McCluskey M D 2020 J. Appl. Phys. 127 101101 Google Scholar
[8]	Zhang J, Shi J, Qi D C, Chen L, Zhang K H L 2020 APL Mater. 8 020906 Google Scholar
[9]	Koksal Q, Tanen N, Jena D, Xing H G, Rana F 2018 Appl. Phys. Lett. 113 252102 Google Scholar
[10]	Varley J B, Weber J R, Janotti A, Van de Walle C G 2010 Appl. Phys. Lett. 97 142106 Google Scholar
[11]	Kananen B E, Halliburton L E, Scherrer E M, et al. 2017 Appl. Phys. Lett. 111 072102 Google Scholar
[12]	Feng Z, Bhuiyan A F M, Kalarickal N K, Rajan S, Zhao H 2020 Appl. Phys. Lett. 117 222106 Google Scholar
[13]	Sun Y F, Li Z G, Fang Y, Wu X Z, Zhou W F, Jia Z T, Yang J Y, Song Y L 2022 Appl. Phys. Lett. 120 032101 Google Scholar
[14]	Zhang Z, Farzana E, Arehart A R, Ringel S A 2016 Appl. Phys. Lett. 108 052105 Google Scholar
[15]	Islam M M, Rana D, Hernandez A, Haseman M, Selim F A 2019 J. Appl. Phys. 125 055701 Google Scholar
[16]	Islam M M, Adhikari N, Hernandez A, et al. 2020 J. Appl. Phys. 127 145701 Google Scholar
[17]	Yamaoka S, Furukawa Y, Nakayama M 2017 Phys. Rev. B 95 094304 Google Scholar
[18]	Gao H, Muralidharan S, Pronin N, et al. 2018 Appl. Phys. Lett. 112 242102 Google Scholar
[19]	Skachkov W R L, Lambrecht H J, von Bardeleben U 2019 J. Appl. Phys. 125 185701 Google Scholar
[20]	Montes J, Kopas C, Chen H, et al. 2020 J. Appl. Phys. 128 205701 Google Scholar
[21]	Othonos A, Zervos M, Christofides C 2010 J. Appl. Phys. 108 124302 Google Scholar
[22]	Singh A, Koksal O, Tanen N, McCandless J, Jena D, Xing H G, Peelaers H, Rana F 2021 Phys. Rev. Res. 3 023154 Google Scholar
[23]	Cho J B, Jung G, Kim K, Kim J, Hong S K, Song J H, Jang J I 2021 J. Phys. Chem. C 125 1432 Google Scholar
[24]	方宇, 吴幸智, 陈永强, 杨俊义, 宋瑛林 2020 69 168701 Google Scholar Fang Y, Wu X Z, Chen Y Q, Yang J Y, Song Y L 2020 Acta Phys. Sin. 69 168701 Google Scholar
[25]	Fang Y, Wu X Z, Yang J Y, Wang J P, Wu Q Y, Song Y L 2021 Appl. Phys. Lett. 118 112105 Google Scholar
[26]	Fang Y, Yang J Y, Yang Y, Wu X Z, Xiao Z G, Zhou F, Song Y L 2015 Journal of Phys. D: Appl. Phys. 49 045105 Google Scholar
[27]	王建苹, 吴幸智, 杨俊义, 陈永强, 吴泉英, 宋瑛林, 方宇 2022 光学学报 42 2219001 Google Scholar Wang J P, Wu X Z, Yang J Y, Chen Y Q, Wu Q Y, Song Y L, Fang Y 2022 Acta Opt. Sin. 42 2219001 Google Scholar
[28]	Singh A, Koksal O, Tanen N, McCandless J, Jena D, Xing H L, Peelaers H, Rana F 2020 Appl. Phys. Lett. 117 072103 Google Scholar
[29]	Chen H, Fu H, Huang X, Montes J A, Yang T H, Baranowski I, Zhao Y 2018 Opt. Express 26 3938 Google Scholar
[30]	Sun Y F, Fang Y, Li Z G, Yang J Y, Zhou W F, Liu K, Song Y L 2021 J. Phys. D: Appl. Phys. 54 495105 Google Scholar
[31]	Kuramata A, Koshi K, Watanabe S, Yamaoka Y, Masui T, Yamakoshi S 2016 J. Appl. Phys. 55 1202A2 Google Scholar
[32]	Luchechko A, Vasyltsiv V, Zhydachevskyy Y, et al. 2020 J. Phys. D: Appl. Phys. 53 354001 Google Scholar
[33]	Galazka Z, Ganschow S, Fiedler A, et al. 2018 J. Cryst. Growth 486 82 Google Scholar
[34]	Peelaers H, Van de Walle C G 2019 Phys. Rev. B 100 081202 Google Scholar
[35]	Varley J B, Peelaers H, Janotti A, Van de Walle C G 2011 J. Phys. Condens. Matter 23 334212 Google Scholar
[36]	Deák P, Ho Q D, Seemann F, Aradi B, Lorke M, Frauenheim T 2017 Phys. Rev. B 95 075208 Google Scholar
[37]	Ingebrigtsen M E, Kuznetsov A Y, Svensson B G, Alfieri G, Mihaila A, Badstübner U, Perron A, Vines L, Varley J B 2019 APL Mater. 7 022510 Google Scholar
[38]	Johnson J M, Chen Z, Varley J B, et al. 2019 Phys. Rev. X 9 041027 Google Scholar
[39]	Nie Y Y, Jiao S J, Li S F, et al. 2022 J. Alloys Compd. 900 163431 Google Scholar
[40]	Farzana E, Ahmadi E, Speck J S, Arehart A R, Ringel S A 2018 J. Appl. Phys. 123 161410 Google Scholar
[41]	Zimmermann C, Rønning V, Frodason Y K, Bobal V, Vines L, Varley J B 2020 Phys. Rev. Mater. 4 074605 Google Scholar
[42]	Fang Y, Wu X Z, Yang J Y, Xiao Z G, Yang Y, Zhou F, Song Y L 2015 Appl. Phys. Lett. 107 051901 Google Scholar
[43]	Ščajev P, Jarašiūnas K, Leach J 2020 J. Appl. Phys. 127 245705 Google Scholar
[44]	Reshchikov M A, Vorobiov M, Demchenko D O, et al. 2018 Phys. Rev. B 98 125207 Google Scholar

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Broadband ultrafast photogenerated carrier dynamics induced by intrinsic defects in $\boldsymbol\beta$-Ga₂O₃

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Corresponding author: Fang Yu, yufang@usts.edu.cn

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Broadband ultrafast photogenerated carrier dynamics induced by intrinsic defects in $\boldsymbol\beta$-Ga2O3

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Authors and contacts

Corresponding author: Fang Yu, yufang@usts.edu.cn

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Broadband ultrafast photogenerated carrier dynamics induced by intrinsic defects in $\boldsymbol\beta$-Ga₂O₃