Влияние гетеровалентного допирования на структуру и фотостимулированные процессы в галогенидном перовските CsPbBr3 тема диссертации и автореферата по ВАК РФ 00.00.00, кандидат наук Али Ибрагим Мохаммед Шарафелдин

• Али Ибрагим Мохаммед Шарафелдин
• кандидат наук
• 2022

Оглавление диссертации кандидат наук Али Ибрагим Мохаммед Шарафелдин

Table of Contents

Abstract

Introduction

Chapter 1. Literature review

1.1. Basic structure, properties of Perovskite materials and their Applications

1.2. Main characteristics of perovskite materials

1.2.1. Advances and challenges of organic-inorganic and all-inorganic PSCs

1.2.2. Optical properties

1.2.3. The intrinsic Defects in Perovskite

1.2.4. Doping of perovskite

1.2.5. Photoinduced defect formation

1.2.6. Photoluminescence (PL)

Chapter 2. Experimental methods and crystal characterization

2.1. Materials

2.1.1. Synthesis of CsPbBr3 powder

2.1.2. Silver Doped CsPbBr3

2.1.3. Bismuth Doped CsPbBr3

2.2. Characterizations of samples

2.2.1. X-ray powder diffraction (XRD)

2.2.2. Crystal-structure refinement

2.2.3. X-ray photoelectron spectroscopy

2.2.4. Atomic emission spectroscopy

2.2.5. Scanning electron microscope (SEM) and Energy Dispersive X-ray Analysis

2.2.6. Diffuse reflectance spectra

2.2.7. Photoinduced Defect Formation

2.2.8. Luminescence Spectra

2.2.9. Photostimulated photoluminescence quenching

Chapter 3. Effect of heterovalent doping on the structural properties in CsPbBr3 perovskite

3.1. Characterization of silver-doped CsPbBr3 perovskite samples

3.1.1. X-ray diffraction studies of Ag-CsPbBr3 samples

3.1.2. X-ray photoelectron spectra of Ag-CsPbBr3 samples

3.1.3. Scanning electron microscopy and energy-dispersive x-ray analysis for Ag-CsPbBr3 samples

3.2. Bismuth-doped perovskite CsPbBr3

3.2.1. X-ray diffraction studies of Bi-CsPbBr3 samples

3.2.2. X-ray photoelectron spectra of Bi-CsPbBr3 samples

3.2.3. Scanning electron microscopy and energy-dispersive x-ray analysis for Bi-CsPbBr3 samples

3.3. Conclusions to this Chapter

Chapter 4. Photostimulated defect formation of hetrovalent doped CSPbBr3 perovskite

4.1. Study of the optical properties of Ag-CsPbBr3

4.2. Study of the optical properties of Bi-CsPbBr3

4.3. Kinetics of photocoloration of hetrovalent doped CSPbBr3 perovskite

4.4. Conclusions to this Chapter

Chapter 5. Photoluminescence of pristine and doped CsPbBr3 samples

5.1. Photoluminescence of the pristine CsPbBr3

5.2. Photoluminescence of the Bi-doped CsPbBr?

5.3. Photoluminescence of the Ag-doped CsPbBr3

5.4. Conclusion to the Chapter

Conclusion

Acknowledgments

Reference

Введение диссертации (часть автореферата) на тему «Влияние гетеровалентного допирования на структуру и фотостимулированные процессы в галогенидном перовските CsPbBr3»

Abstract

Metal halide perovskite materials have attracted intense interest in the photovoltaic community due to their high efficiency, ease of fabrication, and bandgap tunability. One avenue for improving the PV application is by replacing organic cations with inorganic cations, such as cesium (Cs). The advantage of cesium lead halide perovskite materials is their higher bandgap, which makes them suitable for tandem solar cells, spintronics, light-emitting diodes, lasers, photodetectors, X-ray detectors, and gamma detectors.

The aim of this work is to determine the effect of heterovalent doping on the structural and optical properties of CsPbBr3 perovskite as a promising material for photovoltaic elements.

To achieve the goal of this work the following tasks were solved: (i) investigate the impact of replacing some of the Pb in CsPbBr3 perovskite materials with Ag or Bi on the structure of perovskite; (ii) Study the effect of doping on the structure, optical and luminescent characteristics of the CsPbBr3 halide perovskite and (iii) Investigation of photoinduced defect formation on the photoluminescence of dispersed CsPbBr3.

The synthesis was carried out by the method of precipitation chemistry. Crystallinity, morphology, and optical properties of CsPbBr3 micropowders made were studied and characterized. The main idea is applying to introduce electronic impurities (atomic dopants) into the perovskite materials for tuning the light absorption coefficient, the optical, excitonic, and electrical properties of CsPbBr3 perovskite. This thesis investigated the photophysics of CsPbBr3 on absorption, and photostimulated defect formation of dispersed CsPbBr3 perovskites has been studied by diffuse reflectance spectroscopy. Ag doping does not affect the

fundamental light absorption of CsPbBr3 and does not cause an alteration of the apparent optical band gap. At the same time, Bi doping significantly extends the spectral region of absorption toward the extrinsic absorption spectral region. The study of photocoloration of solids extends a chance to explore both pre-existing and photoinduced defects. Two different mechanisms are realized: typical for both photoresistant and photosensitive solids have been demonstrated by means of physicochemical characterization of the materials and investigations of photoinduced coloration.

The doping with Bi results in strong resistance to photostimulated defect formation. In contrast, the doping with Ag significantly facilitates the photostimulated formation of the new defect states. At a higher degree of doping, Ag-doped CsPbBr3 demonstrates a behavior, which is typical for the photosensitive solids.

Bi doping results in significant quenching of the excitonic luminescence and shift of the luminescence band maximum position toward higher energy, while Ag doping does not change both parameters of the excitonic luminescence. Photoirradiation of the halide perovskite samples leads to the photostimulated luminescence quenching that, in general, correlates with photostimulated formation of the intrinsic defects.

Introduction

Hybrid organo-inorganic perovskites and inorganic perovskites, and perovskite-like materials have attracted significant attention in the scientific community as active components of solar cells due to their optoelectronic and electrophysical properties. Perovskite materials have shown astonishing achievements in perovskite solar cells ( PSCs), which achieved a record certified efficiency of over 25.2% [1]. They are also fascinating for broad applications in spintronics [2], light-emitting diodes [3,4], lasers [4], photodetectors [5-7], X-ray [8], and gamma detectors [9].

Perovskite materials are also easier to fabricate using a simple solution process with earth-abundant chemical species. The criteria to be met by these elements include mainly size restrictions (i.e., tolerance of Goldschmidt and octahedral factor). The fact that several perovskite properties are exceptionally smoothly tunable why the composition is interchangeable [10].

The optoelectronic properties of perovskites offer extreme tenability, low-cost processes, and versatility. Their large absorption coefficient and composition-dependent bandgap make them ideal materials for light-absorbing and emitting applications. Mainly coulombic interactions between the photoexcited electrons and holes give rise to "excitonic effects" that modulate the optoelectronic behaviour of semiconductors [11].

Moreover, their defect tolerant crystal structure (the dominance of shallow point defects) restrains charge carrier recombination processes, and their long carrier diffusion length generates free charge carriers. These qualities are the underlying reasons for the remarkable efficiency of the derived solar cells. The limiting factor

of the commercialization of perovskite materials based devices is their sensitivity towards several environmental factors (e.g., humidity, heat, light) [12].

Although organic-inorganic perovskites have a suitable bandgap for PV application and can obtain high power conversion efficiency (PCE), the organic component volatility in the perovskite film and elsewhere in the device causes thermal instability in PSCs. Incorporating inorganic cations (Cs+) into organic-inorganic perovskites can further improve structural and thermal stability [13]. Even higher thermal stability would be achieved by replacing all the organic cations with inorganic cations [14]. Inorganic Cs-based perovskites have a wider bandgap than their organic counterparts, making them suitable for tandem solar cells, light-emitting diodes (LEDs), and sensors [15].

Thus these materials are appealing for alternative photovoltaic technologies. However, perovskite materials present substantial issues, such as instability to environmental conditions, toxicity (as most of the perovskite materials for PV applications contain lead), and electrical hysteresis. Numerous research groups are focusing on solving these issues [16]. In particular, the stability and hysteresis issues have shown remarkable improvement by using multi-cation mixed halide perovskite materials [17], and it was shown that lead might be replaced with tin for the production of environmentally friendly materials, with fewer issues related to disposal and/or recycling processes [18]. Therefore, the main goal of the perovskite research community is to fulfill the "golden triangle" of solar cell technology, this being cost, efficiency, and stability properties for the fast commercialization of the product.

The aim of this work was to study the effect of heterovalent cation doping on the structure and optical properties of perovskite materials. In order to achieve this goal, the following problems were to be solved:

1. Synthesis of nominally pure and doped Ag+ and Bi3+ micro dispersed samples of CsPbBr3.

2. Physico-chemical characterization of the synthesized samples to establish their structure and elemental composition.

3. Investigation of the effect of doping on the optical and luminescent characteristics of the CsPbBr3 halide perovskite.

4. Investigation of the processes of photoinduced defect formation and the effect of doping on the efficiency of processes.

5. Investigation of the effect of doping and photoinduced defect formation on the photoluminescence of dispersed CsPbBr3.

To solve these problems, the following research methods were selected. The effect of adding a small amount of Ag+ or Bi3+ cations in inorganic perovskite upon doping was considered. The study of the effect of photoinduced defect formation using diffuse reflectance spectroscopy was applied to analyze the samples' defective structure. We also examine the nature of the photoluminescence quenching and charge transfer properties between the cations doping either Ag+ (p-type) or Bi3+ (n-type) and pristine CsPbBr3 perovskite. Finally, the samples' comprehensive physicochemical characterization was carried out by the following methods:

• X-ray diffraction analysis

• Scanning electron microscopy

• X-ray photoelectron spectroscopy

• Luminescent technique

• Diffuse reflectance spectroscopy

The reliability and approbation of the research. The reliability of the results obtained is provided by the use of modern physicochemical research methods for studying the perovskite structure, reproducibility of experimental results, and the consistency of data obtained for perovskite materials exposed to light-irradiation with known literature data.

The research results were published in peer-reviewed journals[19-22]:

1) Ibrahim M. Sharaf, Anna V. Shurukhina and Alexei V. Emeline, Structural and Optical Properties of Pristine and Doped CsPbBr3 Perovskite, IOP Conf. Series: Earth and Environmental Science 706 (2021) 012044. https://iopscience.iop.org/article/10.1088/1755-1315/706/17012044

2) Ibrahim M. Sharaf, Anna V. Shurukhina, Irina S. Komarova and Alexei V. Emeline, Effect of heterovalent doping on photostimulated defect formation in CsPbBr3, Mendeleev Commun., 2021, Vol. 31, issue 4, p. 465-468, https: //www. doi.org/%2010.1016/j.mencom.2021.07.009

3) Vyacheslav N. Kuznetsov, Nadezhda I. Glazkova, Ruslan V. Mikhaylov, Ibrahim M. Sharaf, Vladimir K. Ryabchuk, Alexei V. Emeline, and Nick Serpon, Separation and Recombination of Photocarriers from Color Centers and Optically Silent Trap States from 100 to 450 K: The Halide Double Photochromic Perovskite Cs2AgBiBr6, ACS Appl. Mater. Interfaces, 21, 13, 21, 25513-25522 , https://pubs.acs.org/doi/pdf/10.1021/acsami.1c03721

4) Ibrahim M. Sharaf, Anna V. Shurukhina, Irina S. Komarova and Alexei V. Emeline, Photoinduced defect formation in pristine and doped CsPbBr3 perovskite, Journal of Xi'an University of Architecture & Technology,

Volume XI, Issue XII, 2019, https://www.xaj zkj dx.cn/gallery/62-dec2019.pdf

The results of the work were reported at the following scientific conferences:

1) Emeline A. V., Komarova I. S., Sharaf I., Photostimulated defect formation in pristine and doped halide perovskites, in: conf. MAPPIC-2019, October 14-15, 2019 Moscow, Russia, P-18.

2) Ibrahim Sharaf, Anna Shurukhina, Irina Komarova, Alexei Emeline, photoinduced defect formation of pristine and doped CsPbBr3 perovskite, in: Conf. ICESS 2020, 9-10 January, 2020, Saint Petersburg , Russia, p 15.

3) Sharaf I. M., Shurukhina A., Komarova I., Emeline A., Photostimulated Defect Formation in Doped and Undoped CsPbBr3 Perovskite, in: conf. MAPPIC-2020, 26-28 October 2020. Moscow, Russia, P-73.

4) Ibrahim M Sharaf, Alexei V. Emeline, Photoinduced defect formation in pristine and doped CsPbBr3 perovskite, in: Conference "Science and Progress", November 10-12, 2020. Saint-Petersburg State University (Saint-Petersburg, Russia).

5) Ibrahim M. Sharaf, Alexei V. Emeline" Photoinduced color center formation in pristine and doped CsPbBr3 perovskit" in: Conference Наука СПбГУ - 2020, December 24, 2020, Saint-Petersburg, Russia.

6) Ibrahim M. Sharaf, Anna V. Shurukhina, Alexei V. Emeline, Structural and optical properties of pristine and doped CsPbBr3 perovskite, in: Conf. GMEE2021, February 2-3, 2021 , Changsha, China.

The scientific novelty of the results:

1. the systematic studies of the type and concentration of heterovalent dopant on the structure of CsPbBr3 halide perovskite.

2. the effect of heterovalent dopant types and contents on photostimulated defect formation.

3. the intrinsic defect states redistribution is determined by the type and concentration of heterovalent dopants.

4. Correlation between the efficiency of photostimulated defect formation in doped halide perovskite and degree of the lattice distortion.

5. Dependence of either photoresistant or photosensitive type of halide perovskite on the type and concentration of the heterovalent dopants.

6. Correlation between dopant induced luminescence quenching and the number of the intrinsic compensating defects

7. Correlation between photostimulated luminescence quenching and the number of photoinduced defects.

Thesis statements to be defended:

1. Heterovalent doping of CsPbBr3 halide perovskite results in lattice distortion dependent on the type and concentration of the dopants.

2. Monovalent and trivalent cation doping leads to stabilization of intrinsic compensating defects, which type and their spectral and energy distributions are determined by the type and concentration of the dopants.

3. Characteristics and mechanisms of photostimulated defect formation depend on the type and concentration of the heterovalent dopants.

4. Mechanisms of the excitonic luminescence quenching are determined by the type and concentration of the intrinsic defects.

5. Correlations between structural parameter (lattice volume) and efficiency of photostimulated defect formation and excitonic luminescence band characteristics.

The author's personal contribution was conducting experimental studies, processing and interpreting data obtained by spectral methods, analyzing the results obtained, as well as writing articles, and preparing reports on the results of research.

The personal contribution of the author. The author with Anna Shurukhina were synthesized a series of Ag+ and Bi3+ samples of doped CsPbBr3 perovskites. Samples characterization was carried out with technical support by resource centers "Nanophotonics", "X-ray Diffraction Studies", "Physical Methods of Surface Investigation", "Centre for Geo-Environmental Research and Modelling (GEOMODEL)", "Chemistry Educational Centre", "Innovative technologies of composite nanomaterials", and "center for Optical and Laser Materials Research" of the Research Park of St. Petersburg State University, analysis of the results was carried out by the author. The author personally obtained all results on absorption, photoluminescence quenching, and photoinduced coloration of defects. Results and conclusions were discussed with the supervisor. Together with co-authors and the supervisor, the authors were conducting experimental studies, processing and interpreting data obtained by spectral methods, analyzing the results obtained, writing articles, and preparing reports on research results.

Заключение диссертации по теме «Другие cпециальности», Али Ибрагим Мохаммед Шарафелдин

Заключение

В заключение, на основании полученных в работе основных результатов можно сделать следующие выводы:

1. Синтезированы два набора перовскита CsPbBr3, допированного Вь и Ag, с содержанием Ag 0,0 ат%, 0,038 ат%, 0,088 ат%, 0,29 ат% и 0,44 ат%, и Bi 0,0 ат%, 0,088 ат%, 0,18 ат%, 0,26 ат% и 0,43 ат%.

2. Образцы перовскита CsPbBr3 кристаллизуется в орторомбической фазе перовскита. Введение контролируемых примесей Ag или Bi не приводит к изменению фазового состава.

3. Гетеровалентное допирование перовскита СбРЬБгз приводит к изменению объема элементарной ячейки. Характер изменения зависит от типа и концентрации допантов. Допирование Ag и Bi сохраняет стабильность параметра решетки.. Допирование как Ag, так и Bi поддерживает стабильность параметра решетки.

4. Допирование Ag не влияет на фундаментальное поглощение света CsPbBr3 и не приводит к изменению оптическоой ширины запрещенной зоны (2,26 эВ). В то же время, допирование Bi значительно расширяет спектральную область поглощения, вызванную образованием дефектных состояний.

5. Допирование Bi или Ag приводит к перераспределению собственных дефектов и образованию доминирующих типов дефектных состояний в зависимости от типа и концентрации допанта для компенсации избытка заряда соответствующих катионов допанта, что приводит к различным типам собственных дефектов.

6. Фотовозбуждение перовскитных материалов в области собственного поглощения приводит к образованию фотоиндуцированных дефектов. Этот эффект фотоиндуцированного дефектообразования высокоэффективен для

образцов, содержащих серебро. Образование дефектов в перовскитовых материалах, содержащих висмут, низкоэффективно.

7. Допирование Bi приводит к повышению устойчивости к фотостимулированному дефектообразованию, тогда как допирование Ag значительно облегчает фотостимулированное образование новых дефектных состояний и при более высокой степени допирования Ag-допированный СбРЬБгз демонстрирует поведение, характерное для фоточувствительных твердых тел.

8. Допирование Bi приводит к значительному тушению экситонной люминесценции и смещению положения максимума полосы люминесценции в сторону более высоких энергий, в то время как Ag=допирование не изменяет оба параметра экситонной люминесценции.

9. Допирование Ag и Bi приводит к изменению параметра FWHM полосы люминесценции, и его изменения коррелируют с изменениями объема ячейки, вызванными допированием.

10. Фотооблучение образцов галогенидного перовскита приводит к фотостимулированному тушению люминесценции, что в целом коррелирует с фотостимулированным образованием внутренних дефектов.

На основании полученных результатов можно сделать следующие выводы:

1. Гетеровалентное допирование не влияет на кристаллическую структуру галогенидного перовскита CsPbBr3, однако нарушает решетку, что приводит к изменению объема ячейки в зависимости от концентрации допирующего элемента.

2. Гетеровалентное допирование Ag+ и ВР+ приводит к образованию внутренних дефектов, компенсирующих избыток заряда допирующих катионов. Внутренние дефекты, индуцированные Вьдопированием, оптически активны и ответственны за расширение края поглощения в

эксктринную область спектра поглощения, в то время как внутренние дефекты, индуцированные Ag-допированием, изначально оптически неактивны и становятся оптически активными при облучении за счет фотогенерации носителей заряда.

3. Увеличение концентрации допирующих элементов приводит к перераспределению собственных дефектов и стабилизации определенного типа собственных дефектов в зависимости от типа и концентрации допирующих элементов.

4. Эффективность фотостимулированного дефектообразования в галогенидных перовскитах CsPbBr3, допированных Ag и В^ коррелирует с изменением объема решетки, вызванным допированием, что указывает на степень искажения кристаллической структуры.

5. Характер кинетики фотостимулированного дефектообразования в нетронутом и Вьдопированном галогенидном перовските CsPbBr3 соответствует фотоустойчивым твердым телам и указывает на то, что механизм фотостимулированного дефектообразования обусловлен захватом носителей заряда предсуществующими дефектными состояниями.

6. Увеличение концентрации допирующего элемента Ag приводит к трансформации кинетики фотостимулированного дефектообразования от кинетики, характерной для фотоустойчивых твердых тел, к кинетике, характерной для фоточувствительных твердых тел, что в свою очередь свидетельствует об изменении доминирующего механизма фотостимулированного дефектообразования.

7. Изменения параметра FWHM полосы люминесценции при увеличении концентрации допирующих веществ коррелируют с изменением объема ячейки под действием допирующих веществ и могут быть объяснены неоднородным браденированием экситонной люминесценции.

8. Тушение люминесценции, вызванное увеличением концентрации допанта В^ коррелирует с увеличением числа компенсирующих внутренних дефектов. Механизм тушения связан с распадом экситонов на компенсирующих внутренних дефектах.

9. Фотостимулированное тушение люминесценции связано с фотостимулированным образованием дефектных состояний и может быть приписано распаду экситонов на фотоиндуцированных дефектах.

10. Внутренние дефекты, компенсирующие избыток заряда в Вь допированных образцах, и фотоиндуцированные дефекты в Ag-допированном галогенидном перовските могут быть отнесены к междоузельным Вг-состояниям.

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