152 IEEE TRANSACTIONS ON ELECTRON DEVICES, VOL. 69, NO.

1, JANUARY 2022

Praseodymium-Doped In-Sn-Zn-O TFTs With

Effective Improvement of Negative-Bias
Illumination Stress Stability
Hengbo Zhang, Lingyan Liang , Xiaolong Wang, Zhendong Wu , and Hongtao Cao

Abstract — In this work, amorphous praseodymium- In-Sn-Zn-O (ITZO) TFTs present the potential of high μFE
doped In-Sn-Zn-O (ITZO-Pr) thin-film transistors (TFTs) (>20 cm2 · V−1 · s−1 ) and have been widely studied in recent
were fabricated with improved negative-bias illumination years [4]–[7]. In3+ and Sn4+ have similar 5-s orbitals [8].
stress (NBIS) stability under different radio frequency (RF)
magnetron sputtering powers. The optimized ITZO-Pr TFTs By partially replacing In with Sn, the cost of TFT fabrication
presented field effect mobility (μFE ) of 20.9 cm2 · V−1 · s−1 , can be reduced. On the other hand, tin oxide-containing
steep subthreshold (SS) of 0.27 V/dec, and small threshold materials have high resistance to conventional acids and
voltage shift (Vth = −2.12 V) under NBIS (−20 V, 3600 s). alkalis [9], which helps achieve etch-stop-layer-free processes.
All Pr-doped devices exhibited a reduction in light respon- Nevertheless, ITZO TFTs exhibit obvious instability under
sivity of more than one order of magnitude compared with
ITZO TFTs. Moreover, after Pr doping, relaxation processes negative bias illumination stress (NBIS) since ITZO is more
of photoelectrons changed and then the activation energy sensitive to visible light compared to IGZO [10], [11].
(Ea ) of light-induced electrons relaxation decreased, which The most general method to enhance stability is to suppress
enhanced the NBIS stability of ITZO TFTs effectively. the formation of oxygen vacancies (VO ) by doping elements
Index Terms — Amorphous oxide semiconductors that have strong binding energy with oxygen [12]–[14] or to
(AOSs), flat panel displays, rare earth element doping, increase the energy required for VO excitation by widening
thin-film transistors (TFTs). the optical bandgap (E g ) [15]. Nevertheless, VO is an intrinsic
defect in AOS and cannot be eliminated thoroughly. Recently,
I. I NTRODUCTION a new method for improving light stability has been proposed
via doping praseodymium (Pr), as illustrated in In-Zn-O
A MORPHOUS oxide semiconductor (AOS) has gradually
replaced traditional channel materials of thin-film tran-
sistors (TFTs) used in flat panel displays such as hydrogenated
TFTs [16] and In-Ga-O TFTs [17]. A trap-assisted recom-
bination center hypothesis was proposed in these articles.
amorphous silicon (a-Si: H) and low-temperature polycrys- However, further investigations are required in order to verify
talline silicon (LTPS) [1]. However, with the demand for the universality and detailed mechanisms of Pr-doping effects
ultrahigh resolution and frame rate, the field effect mobility on AOS TFTs.
(μFE ) of TFTs needs to be further improved [2]. Typical μFE In this work, we compared the electrical performance of
of In-Ga-Zn-O (IGZO) widely used in industry is around ITZO TFTs with and without Pr doping. Significant refinement
10 cm2 /V · s [3], which may not meet the requirement for of NBIS instability has been discovered in ITZO-Pr TFTs
novel displays. Therefore, finding a suitable channel material fabricated under different magnetron sputtering powers. The
with good performance is an emergency issue. stability improvement mechanism of Pr doping was systemat-
ically studied on two kinds of devices/films.
Manuscript received September 27, 2021; revised October 30, 2021;
accepted November 3, 2021. Date of publication November 18, 2021;
date of current version December 29, 2021. This work was supported
in part by the International Cooperation Key Project, in part by the
II. E XPERIMENTAL
Bureau of International Cooperation of the Chinese Academy of Sci- Bottom-gate structure TFTs were fabricated on highly
ences under Grant 174433KYSB20180050, in part by the Natural Sci-
ence Foundation of Zhejiang Province under Grant LD21F040002 and doped p-type Si substrate with a 100-nm-thick SiO2 layer
Grant LY20F010002, and in part by Ningbo Public Service Technol- serving as the gate electrode and insulator, respectively. Two
ogy Foundation, China, under Grant 202002N3156. The review of this different types of 30-nm-thick active layers were separately
article was arranged by Editor J. F. Conley. (Corresponding authors:
Lingyan Liang; Hongtao Cao.) deposited from the ITZO target and ITZO-Pr target (Pr =
The authors are with the Laboratory of Advanced Nano Materials 2 wt.%, the raw material is Pr6 O11 , containing Pr3+ and Pr4+ )
and Devices, Ningbo Institute of Materials Technology and Engineering, by radio frequency (RF) magnetron sputtering at room tem-
Chinese Academy of Sciences, Ningbo 315201, China, and also with
the Center of Materials Science and Optoelectronics Engineering, Uni- perature. The atomic ratio of In/Sn/Zn is 1/2/2. During active
versity of Chinese Academy of Sciences, Beijing 100049, China (e-mail: layer deposition, the RF power (PRF ) applied to the targets was
[email protected]; [email protected]). set at 100, 110, and 120 W, respectively. And the gas flux of
Color versions of one or more figures in this article are available at
https://doi.org/10.1109/TED.2021.3126278. Ar/O2 was fixed at 10/10 sccm. All the films were annealed
Digital Object Identifier 10.1109/TED.2021.3126278 at 350 ◦ C in an air atmosphere for 1 h. The 100-nm-thick

0018-9383 © 2021 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission.
See https://www.ieee.org/publications/rights/index.html for more information.

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ZHANG et al.: PRASEODYMIUM-DOPED In-Sn-Zn-O TFTs WITH EFFECTIVE IMPROVEMENT 153

TABLE I
E XTRACTED E LECTRICAL PARAMETERS OF ITZO AND ITZO-P R TFT S

Fig. 1. Transfer ID –VGS characteristics of TFTs with different PRF :

(a) ITZO and (b) ITZO-Pr. The inset in (a) exhibits the top-view micro-
graph of the fabricated devices. (c) Time dependence of ΔVth under
NBIS tests (power density = 2.2 W/m2 ) of two kinds of TFTs at different
PRF . (d) Relationship between NBIS ΔVth of TFTs (PRF = 120 W) and
light power density. The inset in (d) shows the spectrum of the halogen
light source.

InSnO (ITO) layer was deposited by RF magnetron sputter-

ing through a shadow mask as the source/drain electrodes,
defining the devices with the channel width (W )/length (L) of
800/400 μm. The films/devices with/without Pr doping under Fig. 2. Typical monochromatic light response of the TFTs (PRF =
different sputtering powers were labeled as ITZO(ITZO-Pr)/ 120 W): (a) ITZO and (b) ITZO-Pr. (c) Rrel values. (d) Eg values extracted
from Tauc plot (the square of the product of the absorption coefficient and
100(110,120) in the following text. photon energy versus the photon energy, i.e., (αhν)2 versus hν).
The Keithley 4200SCS semiconductor parameter analyzer
was utilized to characterize the electrical performance of TFTs obvious decrease of Vth appears during NBIS tests in ITZO-
in air. The film properties were characterized at room temper- Pr TFTs. The ITZO-Pr/120 TFTs present the smallest Vth
ature by spectroscopic ellipsometry (J. A. Woollam, Lincoln, of −2.12 V. As shown in Fig. 1(d), the effect of improving
NE, USA), X-ray photoelectron spectroscopy (XPS, AXIS stability under NBIS tests (VGS = −20 V, 600 s, PRF = 120
Supra, Kratos, U.K.), and photoluminescence spectrometer W) becomes more and more prominent with increasing light
(PL, Renishaw inVia Reflex, U.K.). power density. The above results demonstrate that Pr doping
has a conspicuous effect on enhancing the NBIS stability.
III. R ESULTS AND D ISCUSSION To clarify the stability improvement mechanism of the Pr
Fig. 1(a) and (b) shows the typical transfer curves of the doping effect, systematic investigations have been made on
ITZO and ITZO-Pr TFTs. Analogous electrical performance two kinds of devices/films. Monochromatic light was applied
is observed in both kinds of devices with various PRF . Nev- to the back channel of devices to probe the photo-response
ertheless, the ON-current of ITZO-Pr TFTs is slightly lower under irradiation at different wavelengths (λ), as illustrated in
than that of ITZO TFTs. The time dependence of threshold Fig. 2(a) and (b). Both types of TFTs almost show no response
voltage shift (Vth , Vth : VGS at ID = 10−8 A) under NBIS to light with λ ≥ 500 nm. And a noticeable photoresponse
tests (VGS = −20 V, 3600 s, halogen light power density = occurs since λ ≤ 450 nm for the ITZO TFTs. In contrast,
2.2 W/m2 , the spectrum is shown in Fig. 1(d) inset) of all 450-nm light induces a minor response in the ITZO-Pr TFTs
the devices is exhibited in Fig. 1(c). Table I summarizes and their photoresponse to other light with shorter λ is also
the extracted electrical parameters and Vth values. Upon distinctly weakened compared to the ITZO TFTs.
varied PRF , ITZO TFTs present relatively high carrier mobility The light responsivity (R = Iph /Popt , Popt is the optical
(∼27 cm2 · V−1 · s−1 ) and commendable subthreshold (sub- power, Iph is the net photocurrent) describes the photoelectric
threshold (SS) ≤ 0.2 V/dec). However, the ITZO TFTs show conversion ability of a device, which is directly proportional to
inferior NBIS stability (Vth of −9.07 to −13.95 V), which the net photoconductivity (σph ) and can be expressed as [19]
is similar to other reports (−7.2 to −18 V) [10], [11]. The
R ∝ σph = eμFE n = (μFE Aτ )ηeF0 /d
optimized stability of ITZO devices occurs under the condition
of 120 W (−9.07 V), which may be due to better film quality where e is the electron charge, n is the density of pho-
under relatively higher PRF [18]. With Pr doping, compared toexcited carriers in cm−3 , η the quantum efficiency (≈1),
with ITZO TFTs, slight degradation has been found in μFE τ the carrier lifetime, A the absorption ratio, F0 the incident
(∼21 cm2 · V−1 · s−1 ) and SS (∼0.27 V/dec), whereas the photon flux, and d the film thickness. Therefore, the difference

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154 IEEE TRANSACTIONS ON ELECTRON DEVICES, VOL. 69, NO. 1, JANUARY 2022

indicate that the NBIS improvement by Pr doping cannot

be well explained by those two factors but by some new
mechanism related to Pr.
To further investigate the Pr-doping effect, the effective
density of states (DOS) associated with photoexcited states is
extracted from the time decay behaviors of σph after turning
off the 350-nm-wavelength light illumination [20]. The decay
curves are fit by three exponential terms, and the details
of extracted method have been described in our previous
reports [25], [26]. As shown in Fig. 3(c), the differences
of effective DOS between ITZO and ITZO-Pr are much
greater than that from varied RF powers. After Pr doping,
the peak values of effective DOS decrease from the order
of 1019 to 1014 cm−3 · eV−1 . The photoexcited effective DOS
values of ITZO-Pr are comparable to those of IGZO [20],
showing good practical application of Pr-doped ITZO TFTs.
The pronounced suppression of effective DOS indicates that
Fig. 3. (a) XPS spectra of Pr 3d in ITZO and ITZO-Pr films (PRF =
120 W). (b) Relative amounts of VO extracted from O 1s XPS spectra.
Pr doping effectively assists photogenerated carriers’ recombi-
(c) Light-induced effective DOS extracted from the time decay behaviors nation and then reduces the amount of residual light-induced
of σph . (d) PL spectra of ITZO and ITZO-Pr films (PRF = 120 W). The defects (such as VO2+ and VO+ ). Moreover, the corresponding
inset is the room temperature PL spectra of Si and quartz substrate.
activation energy (E a ) of relaxation processes (obtained at
the peak locations of effective DOS) in ITZO and ITZO-Pr
of R between ITZO and ITZO-Pr depends on the product TFTs are ∼1.26 and 0.94 eV, respectively. It should be
of μFE Aτ . In order to exclude the influence of μFE that pointed out that the E a extracted from the decay behavior of
is naturally dissimilar between ITZO and ITZO-Pr, relative photoconductivity is not equal to the energy gap between the
responsivity (Rrel = R/μFE ) is presented to represent the trap level and the conduction band minimum or valence band
photo-response of devices under various monochromatic light maximum. In fact, it reflects the extra energy required for the
irradiation, as depicted in Fig. 2(c). Compared with ITZO photoelectrons’ relaxation process due to the photoreduction
TFTs, the Rrel values of all the Pr-doped devices are reduced effect [20] or the lattice relaxation [26]. Anyway, a smaller E a
by more than one order of magnitude in the whole measured indicates a smaller τ , and thus an easier and quicker relaxation
range (300–450 nm), indicating the overall effect of Pr doping process of the light-induced electrons after Pr doping [27].
on the photo-response not related to the λ values. And the PL measurements (He-Cd laser light, λ = 325 nm) were
ITZO-Pr/120 TFTs present the smallest Rrel values among the conducted to 100-nm-thick ITZO and ITZO-Pr films (PRF =
ITZO-Pr devices fabricated under different PRF . 120 W, for example) fabricated on Si rather than quartz
The E g values are extracted from the Tauc plot as shown in (because the former barely produces PL signal but the latter
Fig. 2(d), that is, ∼3.44 and 3.57 eV for ITZO and ITZO-Pr shows strong noise signals in the λ range of 300–800 nm,
films, respectively. Bandgap widening may be one of the the inset of Fig. 3(d)). As shown in Fig. 3(d), the ITZO film
reasons why Rrel of the ITZO-Pr TFTs is suppressed when shows a significant broad emission centered at ∼700 nm which
the photon energy is smaller than E g . However, it is unable is commonly related to VO [28]. In contrast, the PL signal
to explain the Rrel decrease beyond E g (such as 4.13 eV, is weaker and the broad peak is largely suppressed in the
300 nm) owing to comparable A values between the two types ITZO-Pr films. The diminishment of PL signal intensity in the
of films [20]. ITZO-Pr films implies the nonradiative relaxation, correlating
XPS was used to identify the chemical binding states of the to Pr4+ [29], [32]. And the peak centered at ∼630 nm might
ITZO and ITZO-Pr films at room temperature. As shown in relate to Pr3+ (1 D2 -3 H4 ) [30], [31] or down-convert effect [32].
Fig. 3(a), the peaks of Pr 3d at ∼933 and 953 eV are indexed After Pr doping, the relaxation paths of photoelectrons change
to Pr 3d5/2 and Pr 3d3/2 , respectively [21], [22]. Unfortunately, from the VO energy levels to the Pr-related energy level.
Pr3+ and Pr4+ are difficult to be indexed because of very close Some researchers attributed this alteration to trap-assisted
bonded energy [21]. The contents of Pr in ITZO-Pr/100, 110, recovery by Pr4+ ion [16] or nonradiative transition between
and 120 are 2.39%, 2.42%, and 2.25%, respectively, showing the delocalized ligand molecular and the Pr 4 f orbitals [32].
few distinctions. Fig. 3(b) presents the relative amount of VO We also cannot exclude a possibility that Pr ion forms complex
(the peak area ratio of the VO and O 1s) extracted from the O defects by combining with VO , which strongly affect the
1s XPS spectra in two types of materials. The contents of VO neighboring oxygen vacancy site [33] and then decrease the
between ITZO-Pr and ITZO show few differences regardless E a of the relaxation process. In a word, Pr doping quickens
of PRF applied. Nevertheless, the differences in NBIS stability the relaxation of photoelectrons, resulting in the enhancement
are significant. of NBIS stability.
The general explanation of NBIS in AOS TFTs is light- As shown in the above results, Pr doping is indeed a
induced VO ionization [23], [24]. Accordingly, suppressing the novel approach to improve NBIS stability of AOS TFTs by
formation of VO and widening the bandgap are the universal providing a new path for the relaxation of photoelectrons
methods to enhance NBIS stability. However, the above results rather than suppressing VO or widening E g . In addition, the
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ZHANG et al.: PRASEODYMIUM-DOPED In-Sn-Zn-O TFTs WITH EFFECTIVE IMPROVEMENT 155

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