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. 2021 Mar 2;1(4):459–466. doi: 10.1021/jacsau.1c00024

Harvesting High-Quality White-Light Emitting and Remarkable Emission Enhancement in One-Dimensional Halide Perovskites Upon Compression

Yuanyuan Fang †, Tianyin Shao †, Long Zhang †, Laizhi Sui ‡, Guorong Wu ‡, Kaijun Yuan ‡, Kai Wang †,*, Bo Zou †,*
PMCID: PMC8395689  PMID: 34467308

Abstract

graphic file with name au1c00024_0005.jpg

The pressure induced emission (PIE) behavior of halide perovskites has attracted extensive interest due to its potential application in pressure sensors and trademark security. However, the PIE phenomenon of white-light-emitting hybrid perovskites (WHPs) is rare, and that at pressures above 10.0 GPa has never been reported. Here, we effectively adjusted the perovskite to emit high-quality “cold” or “warm” white light and successfully realized pressure-induced emission (PIE) upon even higher pressure up to 35.1 GPa in one-dimensional halide perovskite C4N2H14PbCl4. We reveal that the degree of structural distortion and the rearrangement of the multiple self-trapped states position are consistent with the intriguing photoluminescence variation, which is further supported by in situ high-pressure synchrotron X-ray diffraction experiments and time-resolved photoluminescence decay dynamics data. The underlying relationship between octahedron behavior and emission plays a key role to obtain high-quality white emission perovskites. We anticipate that this work enhances our understanding of structure-dependent self-trapped exciton (STE) emission characteristics and stimulates the design of high-performance WHPs for next generation white LED lighting devices.

Keywords: pressure-induced emission, one-dimensional perovskite, structural distortion, white-light emitting, self-trapped excitons

Introduction

The low-dimensional halide perovskites (LDHPs) as the derivatives of the traditional ABX3 perovskite structure have shown great potential in the optoelectronic field due to their exceptional stability and excellent optical properties.1−6 Recently, the ever-growing interest in LDHPs has made them a promising class of semiconductor materials for next-generation solid-state lighting applications.7−10 However, the development of white perovskite light-emitting diodes (PeLEDs) is limited by the difficulty of obtaining high-quality white perovskite light-emitting layers, which makes their development far behind that of their green and red analogues.11−16 The one-dimensional (1D) metal halide perovskite C4N2H14PbCl4 crystal is identified as the core–shell quantum wire structure which is composed of double edge-sharing octahedral PbCl64– chains coated with organic C4N2H142+ cations. This distinct 1D quantum-well configuration is prone to multiple self-trapped exciton (STE) states triggering the broadband emission.17 Therefore, this structural feature makes it an attractive material for light emission devices. However, with the limited degree of distortion in the structure, it approaches excellent enough white emission properties to fabricate high-performance optoelectronic devices. Consequently, finding an effective strategy to modulate the luminescence of C4N2H14PbCl4 perovskites would be quite beneficial for their practical applications.

As a controllable and predictable way, pressure is highly instructive for modulating the crystal structures and optical properties of perovskites without changing the composition therein.18−24 Recently, scientists began to shift the focus from high-pressure 3D perovskites research to LDHPs.25−29 Notably, the pressure-induced phase transition and band gap structure tuning on LDHPs render the pressure a feasible strategy to optimize its properties.30−32 For example, the series of LDHPs [CnH2n+1NH3]2PbI4 (n = 4, 8, 12) were confirmed to have longer alkylamine cations that lead to less ease of phase transition upon compression;33 (PEA)PbI4 was observed to have a direct–indirect band gap transition at around 5.8 GPa,34 and BA2PbBr4 was found to have a pressure-induced photoluminescence enhancement below 1.0 GPa.35 However, current high-pressure studies on LDPHs focus on the low-pressure region to obtain novel optical properties, and these materials are plagued by emission quenched upon higher pressure, which mostly limits their potential applications in ultrahigh-pressure sensors devices.36−38 Moreover, the pressure responses of white-light-emitting hybrid perovskites (WHPs) remain to be explored. Therefore, the 1D white emission of C4N2H14PbCl4 with a soft lattice makes us expect some totally different photophysical properties upon compression.17

In this work, we report on the optical properties and crystal structures of C4N2H14PbCl4 up to 40.0 GPa. Interestingly, the emission chromaticity of the initial broadband white emissive C4N2H14PbCl4 can be continuously and widely adjusted upon compression. More intriguing is that the C4N2H14PbCl4 crystal exhibited the periodical pressure-induced emission (PIE) phenomenon until 35.1 GPa, which has never been reported in previous PIE systems. This phenomenon not only breaks the traditional thinking that the pressure-induced PL quenching31 and the PIE effect only exist in the low-pressure region,29 but also corrects the misconception that the decrease of crystallinity of perovskite materials will lead to the destruction of optical properties,36 thus further enriching the concept and scope of the PIE phenomenon. Moreover, the excellent properties of materials under ultrahigh pressure are required in aerospace application field and geological engineering. Our results provide a scientific basis for the potential use of such materials in these extreme conditions. Analysis of combined in situ high-pressure synchrotron X-ray diffraction (XRD) and Raman spectroscopy data indicates that apparently structural distortions of both inter- and intraoctahedrons are accompanied by variation of the Pb–Cl–Pb bond. The octahedra distortion degree increase was believed to cause stronger electron–phonon coupling strength and change the multiple STEs state position, corresponding to the unprecedented emission changes of C4N2H14PbCl4. Our results could serve as important basics to guide the synthesis of high-quality white perovskite for application in WLEDs.

Experimental Details

High Pressure

A diamond anvil cell (DAC) with 400 μm diameter culets was used to reach high pressure conditions. A T301 stainless steel gasket with a 125 μm hole and 40 μm thickness served as the sample chamber. The sample was loaded into the sample chamber along with a ruby ball to determine pressure according to the ruby fluorescence technique. In high pressure optical absorption, PL, and XRD experiments, we used silicone oil as a pressure-transmitting medium.

In Situ High-Pressure Optical Measurements

The in situ high-pressure PL measurements were carried out using the 355 nm line of a UV DPSS laser. In situ high-pressure UV–vis absorption measurements were performed by using a deuterium-halogen light source. The fiber spectrometer used is an Ocean Optics QE65000 spectrometer. The PL micrographs of the samples upon compression were taken with a camera (CanonEos 5D mark II) installed on a microscope (Ecilipse TI-U, Nikon). In situ high-pressure Raman spectra were collected by uisng a Raman spectrometer (iHR 550, Symphony II, Horiba Jobin Yvon) with a 785 nm and 10 mW excitation laser.

Results and Discussion

The optical micrographs in Figure 1a clearly reveal that the emission peak maintain distinct changes throughout the compression process. Remarkably, the emission of the C4N2H14PbCl4 crystal is very bright even at 35.1 GPa. The correlated color temperature (CCT) and color-rendering index (CRI) are two important parameters for white emissive materials. The CCT implies the color of white itself actually changes with a change in its color temperature; it used to further define the color of white emission. CRI reflects the color rendering ability of a light source to objects, and CRI over 80 is the better choice for commercial lighting.11 Therefore, we record the Comission Internationale de l’Eclairage (CIE) chromaticity coordinate of the crystal emissions upon continuous compression (Figure 1b). At ambient conditions, the emission has a CIE coordinate of (0.32, 0.39), whose CCT is 6058 K, the alleged “cold” white light for LED lighting fixtures. The broadband emission has a CRI of 80, which needs to be improved for practical applications. When the pressure is increased to 1.6 GPa, the C4N2H14PbCl4 crystal shifts from “cold” white emission to “warm” white emission with a CCT of 4398 K (Figure S1). After that, the emission color transfers to the cold-white emission direction until it reaches the bright bluish-white emission with over 100 × 103 K CCT at 10.5 GPa. Upon further compression, the emission color transfers back to the “warm” white emission with 5544 K CCT at 40.0 GPa. Accompanied by the CCT changes, the CRI was also well modulated (Figure 1c). Despite the decrease from 1 atm to 2.2 GPa, the CRI of the C4N2H14PbCl4 crystal is obviously enhanced upon further compression until it yields excellent high CRI values of 91 at 14.4 GPa. After that, the CRI decreased with increasing pressure to 20.0 GPa. Then, it became stable with CRI values of 83 until 40.0 GPa, which is higher than that in its ambient condition. Therefore, the high-pressure could be used as a powerful means to achieve adjustable large-scale emission chromaticity.

Figure 1.

Figure 1

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(a) PL photographs of C4N2H14PbCl4 crystal upon compression up to 40.0 GPa. (b) Chromaticity coordinates of the emissions as a function of pressure. The pressure range from 1 atm to 1.6 GPa is represented by the orange pentagon dots, while the range of 2.2–10.5 GPa is represented by the blue round dots, and the last range of 10.5–40.0 GPa is represented by the red pentacle dots. (c) Color rendering index (CRI) of the C4N2H14PbCl4 crystal emissions upon compression; the shadow region is because the correlated color temperatures (CCT) saturation and the CRI of the sample cannot be calculated.

Figure 2 shows PL spectra of C4N2H14PbCl4 crystal ranging from 0.0 to 40.0 GPa recorded with an excitation wavelength at 355 nm. Under ambient pressure, C4N2H14PbCl4 has a quite low brightness broadband white emission with a maximum emission peak at 537 nm and a full width at half-maximum (fwhm) of 207.9 nm, whose Stokes shift up to 207.1 nm (Figure 2a and S2a). This broadband emission is demonstrated to be originated from multiple self-trapped excitons (STEs) emission.17 Upon compression to 2.2 GPa, the intensity of the original broadband emission (BE) experienced a slight increase which is ascribed to the slight convergence between the inorganic octahedron and organic cations under mild compression.39 Surprisingly, a new emission (NE) appears with a shorter emission wavelength of 405 nm (∼80 nm Stokes shifts Figure S2b), indicating possible structural variations. Under 355 nm excitation, the intensity of both the NE emission and the BE emission show a linear dependence on the excitation power density up to 4 mW/cm2 (Figure S3), suggesting that both emissions originated from STEs.17 After that, the intensity of the NE peak experiences an obviously continuous increase accompanied by the BE intensity showing a slight increase until 10.5 GPa (Figure 2b and f) which is usually ascribed to the lattice contraction.40 Meanwhile, the NE emission undergoes a continuous red-shift upon compression from 2.1 to 10.5 GPa. This phenomenon maybe governed by the intermolecular interaction of the inorganic octahedron, which is greatly affected the self-trapped states position. This situation is very similar to the negative ion repulsion of ice and water upon compression.41−43 Then, both the BE intensity and NE intensity showed a decrease up to 15.0 GPa (Figure 2c). Intriguingly, the intensity of the NE and BE both re-emerged with a distinctly persistent enhancement until 35.1 GPa (Figure 2d). To date, the phenomenon of the emission intensity increase above 10.0 GPa has never been reported in previous PIE systems; this is the first report of bright broadband white-light emission in LDHPs at 35.1 GPa. Then, the following pressure made both emission peaks start to decrease again until 40.0 GPa (Figure 2e), and the PL intensity is already very weak when the pressure is 60.0 GPa (Figure S4), which could be due to the severe structural deformation caused by deviatoric stress.36 After decompression, the PL spectrum is slightly weaker than the initial state and returns to the original position (Figure S5). These abundant changes can be reproduced in our repeated experiments.

Figure 2.

Figure 2

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(a–e) PL spectra of C4N2H14PbCl4 crystal upon compression up to 40.0 GPa. The black arrows represent the changes of the PL intensity. (f) Evolution of the broadband emission (BE) and new emission (NE) peak maximum intensity as a function of pressure up to 40.0 GPa. The BE emission intensity is denoted as black pentagon dots, while the NE emission intensity is denoted as red round dots.

Moreover, high-pressure absorption experiments were performed to trace the band gap modulation (Figure S6a). At ambient conditions, the crystal C4N2H14PbCl4 shows an absorption edge located at about 330.9 nm.17 The band gap (Eb) of C4N2H14PbCl4 decreases slightly by 0.05 eV when the compression is 1.6 GPa, indicating the feasible organic-to-inorganic approach in the low pressure range.44 After that, the band gap suddenly increases to 3.83 eV at 2.1 GPa, which coincides with the appearance of the new PL peak. And the color of the sample does not change obviously before and after phase transformation. With further compression, the Eb is slightly decreased from 2.2 to 13.0 GPa, then it experiences a faster rate decrease until 40.0 GPa. This decrease is caused by considerable lattice shrinkage and structural distortion upon enough compression (Figure S6b).32

An in situ high-pressure angle-dispersive X-ray diffraction (ADXRD) experiment up to 40.0 GPa was performed to understand the relationship between optical response and structural variations of C4N2H14PbCl4 (Figure 3a). Upon compression, all the diffraction peaks of original phase shifted to higher angles due to a decrease in the volume of unit cell. At 2.0 GPa, the intensity of the first diffraction peak at ∼3.5° corresponding to the Bragg (101) reflection decreased greatly, a new diffraction peak at ∼3.8° corresponding to the Bragg (001) reflection emerged, and the diffraction peaks underwent an apparent redistribution of intensities in the 2θ range of 7–9°, indicating that the sample structure transformed into a new phase (phase II). As the pressure increased further, all the Bragg diffraction peaks shifted to the higher angles without the emergence of new peaks. Especially, from 14.4 to 40.0 GPa, although the intensity of some original reflections decreased and a few bands were broadened, indicating that significant structural distortion occurs, all the peaks did not disappeared, suggesting a long-range order in the crystal structure which may be due to the high electronegativity matching between Cl– and Pb2+ ions. Different from other perovskites, the beginning of amorphization is always observed around 20.0 GPa.18,45−47 Therefore, 1D C4N2H14PbCl4 crystals can be expected to have some optical properties completely different from those of its 1D analogues in a higher-pressure range.36,48

Figure 3.

Figure 3

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(a) Representative XRD patterns of C4N2H14PbCl4 at selected pressures up to 40.0 GPa. (b, c) Crystal structure of C4N2H14PbCl4 before and after phase transition. (d, e) Schematic illustrations of the Pb–Cl–Pb bond angle within the inorganic layer framework before and after the phase transition.

Rietveld refinement results show that the ambient structure of C4N2H14PbCl4 is the orthorhombic space group Imma with lattice parameters a = 14.11(2), b = 5.82(3), and c = 14.55(2) (Figure S7a and Table S1).17 Then, the crystal structure transforms into triclinic space group P–1 with lattice parameters a = 9.96(3), b = 5.83(3), c = 9.55(1), α = 75.34(2), β = 88.92(2), γ = 80.64(3) at 2.5 GPa (Figure S7b and Table S1). At ambient conditions, C4N2H14PbCl4 is a conventional 1D core–shell quantum wire structure, whose inorganic octahedral chains are surrounded by the organic cations (Figure 3b). At 2.5 GPa, the zigzag rotation of PbCl64– octahedra along the c-axis accompanied by the unit cell volume collapse appeared (Figures 3c and S8b). The triclinic C4N2H14PbCl4 shows an obvious anisotropic compression (Figure S8a). To further clarify the changes inside the crystal structure, we represented the varieties of Pb–Cl bond lengths and Cl–Pb–Cl bond angles upon compression (Figures S9 and S10). When pressure was applied to C4N2H14PbCl4, the Pb–Cl–Pb band angle in the bc plane obviously decreased from 175.28°(2) at ambient conditions to 160.69°(3) at 2.5 GPa (Figure 3d and e) accompanied by no obvious changes in the Pb–Cl band length (Figure S9), which identified the serious distortion of the interoctahedral chains. Accordingly, such evolution of the inorganic structure triggers the structure phase transition, which is coincident with the new PL emission emergence and the sudden band gap blue-shift. With further compression, the interoctahedron became more distorted as the Pb–Cl–Pb bond angle continuous decrease (Figure S10). Meanwhile, the Pb–Cl bond lengths are defined as L1 and L2 also slowly decreased showing the onset distortion of intraoctahedral structures. When the pressure reached 14.7 GPa, the intraoctahedron shrank severely, which triggers the distinct contraction rate of the L1 bond length and L2 bond length (Figures S9 and S11). This is consistent with the PL intensity re-enhancement in the high pressure range. To further study the evolution of the inorganic sublattice layer, we also carried out high-pressure Raman experiments (Figure S12). The Raman spectra confirmed the structural phase transition at 2.3 GPa and the serious structural distortion above 14.6 GPa.

Analysis of combined in situ high-pressure PL, absorption, and time-resolved PL decay dynamics data indicates that the pressure-induced variation of the fascinating optical properties in the C4N2H14PbCl4 perovskite crystal is possibly ascribed to the multiple radiative self-trapped states transformation.17,49

The mechanism of pressure-induced emission in C4N2H14PbCl4 is illustrated in Figure 4a–c. Upon excitation, electrons from the ground state (GS) move into the higher energy free exciton (FE) state and form excited carriers. Although there is an essential difference between the FE state and the free-carrier (FC) state, the changes of the band gaps still contribute to the change of the FE state energy.50,51 The carriers overcome the activation barrier Etrap by thermal activation to realize the transition from the FE states to the multiple STE states or overcome Edetrapn (n = 1,2,3) to bring the carriers on the multiple STE states back to the FE states. Multiple STE states located at various energy states led to STE emission with different wavelengths. When an equilibrium is reached between adjacent STE states, a broad band spectrum is achieved. Under ambient conditions, due to the strong quantum confinement in the initial structure, the excited carriers are easily confined to the conduction band to form bound excitons. The bound excitons can relax to the multiple STE states via the route of the downward dark red arrows (Figure 4a). However, partly bound excitons are easily detrapped from the first STE state back to the FE states (shown by the upward dark red arrow in Figure 4a) due to the much smaller detrap energy barrier Edetrap1 of phase I.17 Therefore, only the self-trapped states with larger Edetrap give emissions in the range around 550 nm (Figure 4a). After 2.0 GPa, the phase transition triggered a sudden increase in the band gap (Figure S6) and the FE state moved to higher position, accompanied by the increase of the Edetrap1 caused the excited carriers in the first STEs no longer detrapped back to the FE state (Figure 3b).52−55 Consequently, a new emission peak emerged located around 390 nm. After that, the marked distorted structure highly increased the electron–phonon coupling and the STE1 state became much lower accompanied by a larger Edetrap activation energy.56 Thus, the emission band in the range 390–420 showed dominating emissions and both emission peaks increase in intensity from 2.0 to 10.5 GPa (Figure S14a). Upon further investigations of PL decay curves at 10.0 GPa, the significantly similar lifetimes of both peaks indicate that both peaks originate from the STE emission (Figure S13a).17 When the STE1 state reaches the deepest place, STE2 and STE3 began to shift to lower positions and there is competition among STE states. Meanwhile, Etrap and Edetrap showed a large enhancement, which promotes the nonradiative recombination of STE excitons via the phonon modes of the huge organic cations (Figure S12b).57 Therefore, although the first emission peak is still at the dominant position, the intensities of both PL peaks decrease continuously with the increase in pressure of 10.5–15.0 GPa. Upon further compression, the position of the STE states will present a reversal where the STE2 and STE3 states become much lower than the STE1 state, which triggers more carriers to be trapped by the STE2 and STE3 states (Figure 4c). Due to the wavelength dependence of STE emission, the decay times can effectively reflect STE state depths; the reversal can be confirmed as shown in Figure S13b. Meanwhile, the obvious intraoctahedral structural distortions not only trigger the distinct band gap decrease and the FE state and Etrap decrease but also cause a substantial increase in the electron–phonon coupling, resulting in the STE radiative recombination experiencing a great increase (Figures S9 and S11).58 Therefore, the emission band at around 550 nm gives dominating emissions and the intensity of both emission peaks increases from 15.0 to 35.1 GPa.

Figure 4.

Figure 4

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Illustrations of PIE mechanism associated with exciton self-trapping (a) at ambient conditions, (b) upon compression at 2.5 GPa, and (c) upon high pressure at 16.0 GPa. Ground state (GS), free exciton state (FE), free-carrier state (FC), and self-trapped exciton state (STE1, STE2, STE3). Etrap = activation energy for self-trapping; Edetrap = activation energy for detrapping.

Conclusion

In conclusion, we have demonstrated an unusual pressure-driven optical response and phase transition in 1D halide perovskite C4N2H14PbCl4. The results show that PL colors of the broadband STE emission can be easily adjusted between “cold” white light and “warm” white light accompanied by higher CRI. In particular, C4N2H14PbCl4 shows a never acquired remarkable PIE phenomenon in the high-pressure area (15.0–35.1 GPa). In situ high-pressure ADXRD and the time-resolved PL decay dynamics data show that the distortions of inorganic octahedral chains and the [PbCl6]4– intraoctahedral unit effectively influence the FE state and STE state position and electron–phonon coupling, which caused the tunable emission chromaticity and STE emission enhancement. This work not only breaks the conventional thinking that the PIE phenomenon only appears in low pressure areas but also provides greater possibility for synthesizing perovskite materials ideal for practical lighting applications.

Supporting Information Available

The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacsau.1c00024.

  • Details of the sample preparation and some experiment details; CCTs at selected pressures; absorption and emission spectra; PL spectra; high-pressure UV/vis absorption spectra; Rietveld refinement and cell parameters; lattice constants and experimental volumes; octahedral chain view of C4N2H14PbCl4; calculated pressure-driven bridging Pb–Cl–Pb angle and Pb–Cl bond length evolution; selected Raman spectra; (PDF)

Author Contributions

We thank L.S., G.W. and K.Y. for assistance with the time-resolved PL decay dynamics measurements. Y.F., T.S., and L.Z. performed high pressure optical and XRD experiments. L.S., G.W., and K.Y. carried out the time-resolved PL decay dynamics measurements. Y.F., K.W., and B.Z. wrote the manuscript. All authors discussed and commented on the manuscript.

This work is supported by the National Science Foundation of China (NSFC) (Nos. 21725304,11774120). The Graduate Innovation Fund of Jilin University. The Chemical Dynamics Research Center (Grant No. 21688102), the Key Technology Team of the Chinese Academy of Sciences (Grant No. GJJSTD20190002). Angle-dispersive XRD measurement was performed at the 4W2 HP-Station, BSRF.

The authors declare no competing financial interest.

Supplementary Material

au1c00024_si_001.pdf (1.1MB, pdf)

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