of PMN-PT 3
Cite as: Appl. Phys. Lett. 119, 252903 (2021); https://doi.org/10.1063/5.0068936
Submitted: 28 August 2021 • Accepted: 03 December 2021 • Published Online: 20 December 2021 Nannan Liu, Zeen Zhao, Wenxiu Gao, et al.
Giant modulation of photoluminescence in CsPbBr 3 films through polarization
switching of PMN-PT
Cite as: Appl. Phys. Lett.119, 252903 (2021);doi: 10.1063/5.0068936 Submitted: 28 August 2021
.
Accepted: 3 December 2021.
Published Online: 20 December 2021
NannanLiu,1 ZeenZhao,1WenxiuGao,1YajunQi,2XinpingZhang,1,a)GuoliangYuan,1,a) and Jun-MingLiu3 AFFILIATIONS
1School of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing 210094, China
2School of Materials Science and Engineering, Hubei University, Wuhan 430062, China
3National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, China
a)Authors to whom correspondence should be addressed:[email protected]and[email protected]
ABSTRACT
CsPbBr3 shows excellent photoelectric properties such as a direct bandgap of 2.25 eV, large optical absorption coefficient, and strong luminescence intensity. Therefore, it is promising to be applied in LED devices. It is important to modulate and enhance photoluminescence (PL) intensity through external stimulus. Here, (001) CsPbBr3films with nanocrystals were grown on the PMN-PT ferroelectric single crystal substrate, and itsPLcan be largely modulated by the ferroelectric polarization switching of PMN-PT. The saturated polarization of a 90 nm thick CsPbBr3film induces a 67% increase in thePLintensity, which is due to piezoelectric strain passivated defects, resulting in decreased nonradiative recombination. However, the upward saturated polarization of the 40 nm thick CsPbBr3film introduces a 55% decrease in the PLintensity, which can be attributed to the inner electric field separating the light-excited electron–hole pairs, thereby decreasing their radia- tive combination. This reversible and tunable photoluminescence is important for the development of advanced multifunctional optoelectri- cal devices.
Published under an exclusive license by AIP Publishing.https://doi.org/10.1063/5.0068936
Hybrid perovskites (HPs) have attracted enormous attention due to their special optoelectronic characteristics,1and all-inorganic perov- skite cesium lead halides (CsPbX3, X¼ Cl, Br, or I) have attracted much attention in light-emitting diodes (LEDs),2–4 x-ray imaging,5 lasers,6,7 and photodetectors.8–10 CsPbBr3 has a direct bandgap of 2.25 eV and large optical absorption coefficient in the visible band.11 Meanwhile, CsPbBr3has a variety of merits such as high photolumi- nescence intensity and large carrier diffusion length,11which implies that CsPbBr3 would have a promising application in photoelectric devices. Furthermore, the colloidal CsPbBr3nanocrystals show high photoluminescence quantum yields and wide tunable bandgap in the visible range, which are desirable properties for light emitting applica- tions.12It is well recognized that large and reliable manipulation of physical properties underlies the operation of many optoelectronic technologies such as electrically pumped lasers and optical wave- guides.13–15The tunability can be accomplished in various ways such as the substitution of ions,16–18quantum confinement of nanocrys- tals,12,19–21heterojunction fabrication,22and modulation of thePLvia bandgap engineering or porous templates.22,23 The electric bias
modulation of the PL is still small for CsPbBr3devices nowadays though it is particularly appealing.
Recently, the electric field-induced modulation of physical prop- erties has been achieved in perovskite-structured semiconductors.24–26 A PMN-PT single crystal substrate possesses large piezoelectric coeffi- cient (d33>2000 pC/N) and high electromechanical coupling factor (k33>0.9). It is noticeable that the electric controlled strain generated from PMN-PT has been utilized to tune electric, magnetic, and optical properties of various materials in previous studies.27–30In a pioneering work, the near-infrared luminescence of the Ni-doped SrTiO3film grown on the PMN-PT substrate was modulated via the converse pie- zoelectric effect induced by an external electric field (Eex).31 The dynamic modulations of photoelectronic properties throughEexadd a new freedom to develop optoelectroic devices and optical communica- tion devices. In a previous work, Renet al.32reported the electric bias- tunedPLof MAPbI3films on PMN-PT substrates.
In this paper, a series of (001) CsPbBr3films with thicknesses from 40 to 200 nm were grown on the (001) PMN-PT single-crystal- line substrate. The PL intensity of the 40 nm thick CsPbBr3 film
decreases 55% when the PMN-PT substrate has a polarization toward the CsPbBr3film. However, thePLintensity of the 90 nm thick film increases 67% when a compressive strain is introduced in the CsPbBr3
film due to the saturated polarization of the PMN-PN substrate trig- gered by 10 kV/cm.
The [001] oriented CsPbBr3film composed of nanocrystals was successfully grown on the (001) PMN-PT substrate by PLD. (Details are in experimental section of thesupplementary material.). Kelso et al.33 achieved the epitaxial relation of CsPbBr3 (100) [011] jj SrTiO3(100) [001], where the CsPbBr3crystal cell with the crystal lat- ticea¼b¼0.583 nm rotates 45in-plane in relation to SrTiO3with a0¼b0¼0.391 nm to decrease the lattice mismatch to 5.57% in 2019.
Here, the PMN-PT single-crystal substrate witha0¼b0¼0.405 nm replaces the SrTiO3substrate to achieve the epitaxial relationship of CsPbBr3(100) [001]jjPMN-PT (100) [011] and further decreases the lattice mismatch to 2.32% for most nanocrystals, as shown in Figs. 1(a)and 1(b). A series of CsPbBr3 films were grown on the PMN-PT single crystal by PLD at 1 mJ per laser pulse and 25–200C (i.e., CsPbBr3(1 mJ, 25–200C) films). All CsPbBr3films show the out-of-plane [001] orientation according to XRD patterns [Fig. 1(c)].
The 40 nm thick CsPbBr3(1 mJ, 25C) film is composed of nanocrys- tals (i.e., nanometer-sized quantum dots) and shows the smooth sur- face with a roughnessRaof 1.45 nm [Fig. 1(d)]. Furthermore, the CsPbBr3(1 mJ, 25C) films with 40–200 nm thickness were prepared, and they are composed of nanocrystals and show the smooth surface withRaof2.55 nm (supplementary materialFig. S1). However, the CsPbBr3(1 mJ, 200C) film has a rough surface withRaabout 8 nm owing to the fact that the average size of the crystal grain increases
with an increase in the growth temperature [Fig. 1(e)andsupplemen- tary materialFig. S2).
The steady-state photoluminescence (PL) spectra of these CsPbBr3films were measured to explore the charge extraction abil- ity,34as shown insupplementary materialFig. S3. According to previ- ous studies, CsPbBr3nanocrystals have many advantageous properties and are more suitable forPLapplications than the bulk form as the quantum confinement improves the electrical and optical properties.12 As expected, the CsPbBr3(1 mJ, 25C) film exhibits the strongestPL intensity among our CsPbBr3films grown by PLD at 25–200C with 1–40 mJ per pulse. The average size of nanocrystal grains of the CsPbBr3film increases fast with the growth temperature, so the quan- tum confinement weakens, the wavelength of thePLincreases, and the PL intensity decreases abruptly.35Only CsPbBr3(1 mJ, 25C) films are studied in the following paragraphs.
The crystal lattice of the CsPbBr3film can be effectively modu- lated by theEexupon the PMN-PT substrate due to the inverse piezo- electric effect of PMN-PT. The PMN-PT ferroelectric single crystal is a standard insulator, and its resistance of the PMN-PT single crystal is about 4000 times higher than the 200 nm thick CsPbBr3semiconduc- tor film (supplementary material Fig. S4). Although a high Eex is applied on Au/CsPbBr3/PMN-PT/Au, over 99.99% bias is on the PMN-PT single crystal rather than the CsPbBr3 film. Figure 2(a) shows the XRD patterns of Au/CsPbBr3/PMN-PT/Au samples under 0–10 kV/cm. With the increasingEexalong the [001] orientation, the diffraction angle of the (002) crystal plane shifts to a lower angle for both the PMN-PT substrate and the CsPbBr3film [Figs. 2(b) and 2(c)], suggesting the elongation of crystal latticesc’ andcof PMN-PT
FIG. 1.(a) Au/PMN-PT (001)/CsPbBr3
(001)/Au structure, where the top elec- trode Au is semitransparent. (b) Epitaxial relationship of CsPbBr3 (100) [001] jj PMN-PT (100) [011] for most nanocrys- tals. (c) XRD patterns of the 200 nm thick CsPbBr3film grown at 25–200C with 1 mJ per pulse. (d) and (e) Surface mor- phologies of CsPbBr3 films grown at 25C and 200C, respectively.
and CsPbBr3 according to the Bragg’s law and the Poisson ratio, respectively. When a positiveEexis applied on the PMN-PT substrate, the field will induce an in-plane compressive strain in the PMN-PT substrate via the converse piezoelectric effect,36,37 resulting in the shrinkage ofaandband the elongation ofc. Benefiting from the epi- taxial relationship of CsPbBr3(001)/PMN-PT (001) for most CsPbBr3
nanocrystals, the compressive strain transfers from the PMN-PT sub- strate to these CsPbBr3 nanocrystals, which decreasesaand b and elongatescin the CsPbBr3film.37Bothc0andcincrease with theEex increasing from 0 to 10 kV/cm [Fig. 2(d)], so a maximum compressive strain (e¼(c(V)-c(0))/c(0)) of 0.13% of PMN-PT and 0.09% of the CsPbBr3 film are realized through various 0–10 kV/cm upon the PMN-PT substrate. Since the saturated ferroelectric polarization can switch in the ns scale,38it is possible to realize the fast strain change in the CsPbBr3film through anEexupon PMN-PT.
The dynamic compressive strain induced from the inverse piezo- electric effect of PMN-PT can abruptly enhance thePLintensity of the CsPbBr3film with the thickness ranging from 90 to 200 nm. ThePL intensity abruptly enhances with theEex upon PMN-PT increases from 0 to 10 kV/cm for the CsPbBr3films with the thickness of 90 nm [Fig. 3(a)], 120 nm [Fig. 3(b)], and 200 nm [Fig. 3(c)]. The ratio of the PL intensity change is defined as DPL/PL¼(PL(E)-PL(0)]/PL(0), wherePL(E) andPL(0) are the intensity at anEexand zero electric
field, respectively. The maximumDPL/PLare 67%, 59%, and 46% for the CsPbBr3film with 90, 120, and 200 nm, respectively. Moreover, thePLpeak shows a slight redshift in the 200 nm thickness film with theEexupon PMN-PT increase [the inset inFig. 3(c)], and the redshift may be related to compressive strain in the CsPbBr3 film.39 Furthermore, thePLintensity of the 200 nm thick CsPbBr3film was measured when theEexchanged with the sequence of 0!10!0! 10 kV/cm!0 with 2.5 kV/cm per step, and theDPL/PLvsEexloop is shown inFig. 3(d). In order to explain this phenomenon, the strain vs Eex loop of PMN-PT [Fig. 3(e)] was achieved through analyzing the XRD patterns of the PMN-PT single crystal under 0–10 kV/cm (supplementary materialFig. S5). There is no strong hysteresis charac- teristic,40,41and the piezoelectric strain at 10 or10 kV/cm is about 0.13% and 0.1%.
The dynamic strain introduces defect passivation, extends the lifetime of electron-hole pairs, and increases the PL intensity in the CsPbBr3film. Defects passivation is an effective way to enhance the luminescence properties of the CsPbBr3film.42The 405 nm pump lights excite electron–hole pairs, and their radiative recombination emits photons with518 nm wavelength. However, many defects are the center of non-radiative recombination, where no photons can be emitted.43Lattice strain can passivate the defects that existed in the CsPbBr3 film and, thus, reduce the nonradiative recombination of FIG. 2.(a) XRD patterns of the 200 nm thick CsPbBr3 film grown on PMN-PT (100) under 0–10 kV/cm. Magnified XRD pattern of the (200) planes of (b) the PMN-PT substrate and (c) the CsPbBr3
film. (d) Lattice constantcof the CsPbBr3
film and 1.414c0of PMN-PT as a function of theEexupon the substrate.
photogenerated carriers, leading to the enhancedPL intensity emis- sion.44–48Transient PL spectroscopy is an advantageous method to measure the lifetime of electron-hole pairs after the excitation light stops.46,49,50Such transient PLintensities decay when the Eexupon PMN-PT increases from 0 to 10 kV/cm [Fig. 3(f)], and the lifetimes of electron–hole pairs are 2.98, 4.83, and 5.67 ns for 0, 5, and 10 kV/cm upon PMN-PT through fitting the intensity vs time curves, respec- tively. This suggests that the compressive strain passivated defects, extends the lifetime of light excited electron-hole pairs, enhances the ratio of radiative recombination to all recombination, and finally increases thePLintensity of the CsPbBr3film.45,51
Being different from the PL intensity increasing under anEex
upon the PMN-PT substrate, thePLintensity of the CsPbBr3film with 40–60 nm thickness abruptly decreases when the bias induces an upward saturated polarization toward the film. TheDPL/PLdecreases 55%, 39%, and 25% for the film with 40 nm [Fig. 4(a)], 50 nm [Fig.
4(b)], and 60 nm [Fig. 4(c)] thicknesses. On the contrary, thePLinten- sity slightly increases with the bias inducing a downward saturated polarization against the CsPbBr3film. As shown inFig. 4(d), theDPL/
PLof the 40 nm thick CsPbBr3film increases about 10% and decreases 55% at10 and 10 kV/cm upon PMN-PT, respectively.
The dependence of thePLintensity onEexshould relate to the charge and polarization of CsPbBr3/PMN-PT. The CsPbBr3film has a low density of carriers, and the density of electrons in the conduction
band is a little higher than that of holes, i.e., an n type semiconduc- tor.52When a negativeEexintroduces a downward polarization against the CsPbBr3film, the negative bound charges at the CsPbBr3/PMN- PT interface repulse free electrons to the Au/CsPbBr3 interface [Fig. 4(e)].41Once the electron–holes pairs are excited by incident light near the Au/CsPbBr3interface, the holes are easy to recombine with high-density electrons immediately that increases thePL intensity.53 On the contrary, positiveEexintroduces an upward polarization and the positive bound charges at the CsPbBr3/PMN-PT interface, which depletes most free electrons and introduces the inner electric field (Ein) toward the Au/CsPbBr3interface [Fig. 4(f)].41,54Once electron–hole pairs are introduced under lights near the Au/CsPbBr3interface, they are separated easily by Ein, which decreases the ratio of radiative recombination to all recombination and reduces thePLintensity.
Although both the piezoelectric strain effect (Fig. 2) and the fer- roelectric field effect (Fig. 4) decrease with the increasing thickness of the CsPbBr3 film, the latter decays faster than the former. For the 40 nm thick CsPbBr3films, the ferroelectric field effect is much stron- ger than the piezoelectric strain effect. The free electrons in the con- duction band are no more than the bound charges of ferroelectric saturated polarization. Therefore, the Eex switches polarization and changes bound charges, and the positive bound charges deplete most free electrons at the CsPbBr3/PMN-PT interface and largely decrease thePLintensity.45Free electrons linearly increase with the thickness of FIG. 3.PLspectra of the CsPbBr3film with thicknesses of (a) 90, (b) 120, and (c) 200 nm when an electric field on PMN-PT increases from 0 to 10 kV/cm. The inset in (c) shows a magnifying PL peak. (d) Dependence ofDPL/PLof the 200 nm thick CsPbBr3film on theEexupon PMN-PT. (e) Dependence of the compressive strain of the PMN- PT substrate on theEexupon PMN-PT. (f) Normalized (Nor.)PLdecay curve of CsPbBr3films with 0, 5, and 10 kV/cm upon PMN-PT.
the CsPbBr3film that increasing from 40 to 60 nm, thus more and more free electrons cannot be depleted by positive bound charges of polarization and the absolute value ofDPL/PLbecomes smaller. The ferroelectric field effect decays fast with the increasing thickness of CsPbBr3, and the piezoelectric strain effect is dominant for the 90–200 nm thick CsPbBr3 films. The compressive strain passivates defects and increases the ratio of radiative recombination, so theDPL/
PLis as high as 67% for the 90 nm CsPbBr3film. However, theDPL/
PLbecomes smaller due to the gradual decay of the compressive strain with the thickness increasing from 90 to 200 nm.
In conclusion, a series of (001) CsPbBr3films with nanocrystals and the thicknesses from 40 to 200 nm were grown on the PMN-PT ferroelectric substrate. ThePLintensity of the 40 nm thick CsPbBr3
decreases 55% when the PMN-PT substrate has an upward saturated polarization introduced by 10 kV/cm. The positive bound charge introduces a deplete region, and its inner electric field separates the light excited electron-hole pairs and decreases the radiative combi- nation, i.e., the electrostatic effect. However, this field effect decays fast with increasing film thickness, and it can be ignored in the 90 nm thick CsPbBr3 film. ThePLintensity of this film increases 67% when a compressive strain is introduced in the CsPbBr3film due to the piezoelectric strain of the PMN-PN substrate triggered by 610 kV/cm. It is argued that the compressive strain allows defect passivation so that the radiative recombination and thePLintensity are enhanced.
See thesupplementary materialfor detailed experimental section and characterization of samples, the surface morphologies images, and thePLspectrum of CsPbBr3films under different growth tempera- tures and laser energies, current vs electric field curves of CsPbBr3 films and PMN-PT substrates, and XRD patterns of CsPbBr3/PMN- PT under different bias voltages.
This work was supported by the National Natural Science Foundation of China (Nos. 51790492, 92163210, 11974167, and 61874055 and 51902159) and the Fundamental Research Funds for the Central Universities (No. 30921013108).
AUTHOR DECLARATIONS Conflict of Interest
The authors have no conflicts to declare.
DATA AVAILABILITY
The data that support the findings of this study are available from the corresponding authors upon reasonable request.
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