Quasi-2D Lead Halide Perovskites for Micro- and Nanolasers Enhanced Publication

Quasi-2D Lead Halide Perovskites for Micro- and Nanolasers 准二维铅基钙钛矿微纳激光器 1 2 first-author equal 汪俊（1998-），男，江西景德镇人，硕士研究生，2017年于长春理工大学获得学士学位，主要从事新型光电材料的制备及微纳激光器件的研究。 E-mail：wangjun212@mails.ucas.ac.cn http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598635&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598645&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598641&type= 24.89202881 29.88733673 汪俊 （1998-），男，江西景德镇人，硕士研究生，2017年于长春理工大学获得学士学位，主要从事新型光电材料的制备及微纳激光器件的研究。 E-mail： wangjun212@mails.ucas.ac.cn wangjun212@mails.ucas.ac.cn 1 2 first-author equal 周奉献（1999-），男，湖南湘西人，硕士研究生，2017年于北京理工大学获得学士学位，主要从事钙钛矿复合光电材料的制备与研究。 E-mail：zhoufengxian21@mails.ucas.ac.cn http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598656&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598656&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598656&type= 24.89202881 29.88733673 周奉献 （1999-），男，湖南湘西人，硕士研究生，2017年于北京理工大学获得学士学位，主要从事钙钛矿复合光电材料的制备与研究。 E-mail： zhoufengxian21@mails.ucas.ac.cn zhoufengxian21@mails.ucas.ac.cn 1 2 1 corresp E-mail： huzhiping@ucas.ac.cn E-mail： huzhiping@ucas.ac.cn 胡智萍（1991-），女，河南新乡人，博士，副研究员，2018年于重庆大学获得博士学位，主要从事新型光电材料的制备及光电器件的研究。 E-mail： huzhiping@ucas.ac.cn http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598661&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598672&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598666&type= 24.89202881 29.88732910 胡智萍 （1991-），女，河南新乡人，博士，副研究员，2018年于重庆大学获得博士学位，主要从事新型光电材料的制备及光电器件的研究。 E-mail： huzhiping@ucas.ac.cn huzhiping@ucas.ac.cn 1 2 corresp dujuan@mail.siom.ac.cn dujuan@mail.siom.ac.cn 杜鹃（1980-），女，山东潍坊人，博士，研究员，博士生导师，2007年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超短脉冲激光与功能材料相互作用（具体包括钙钛矿等纳米发光材料制备及器件）的研究。 E-mail： dujuan@mail.siom.ac.cn http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598677&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598686&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598681&type= 24.89202881 29.88732910 杜鹃 （1980-），女，山东潍坊人，博士，研究员，博士生导师，2007年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超短脉冲激光与功能材料相互作用（具体包括钙钛矿等纳米发光材料制备及器件）的研究。 E-mail： dujuan@mail.siom.ac.cn dujuan@mail.siom.ac.cn 2 1 1 2 corresp lengyuxin@siom.ac.cn lengyuxin@siom.ac.cn 冷雨欣（1975-），男，上海人，博士，研究员，博士生导师，2002年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超强超短激光技术发展及其前沿重要应用等方面的研究。 E-mail： lengyuxin@siom.ac.cn http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598689&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598702&type= http://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=37598694&type= 24.89202881 29.88732910 冷雨欣 （1975-），男，上海人，博士，研究员，博士生导师，2002年于中国科学院上海光学精密机械研究所获得博士学位，主要从事超强超短激光技术发展及其前沿重要应用等方面的研究。 E-mail： lengyuxin@siom.ac.cn lengyuxin@siom.ac.cn 国科大杭州高等研究院 物理与光电工程学院， 浙江 杭州　310024 国科大杭州高等研究院 物理与光电工程学院， 浙江 杭州　310024 School of Physics and Optoelectronic Engineering， Hangzhou Institute for Advanced Study， UCAS， Hangzhou 310024， China School of Physics and Optoelectronic Engineering， Hangzhou Institute for Advanced Study， UCAS， Hangzhou 310024， China 中国科学院上海光学精密机械研究所 强场激光物理国家重点实验室， 上海　201800 中国科学院上海光学精密机械研究所 强场激光物理国家重点实验室， 上海　201800 State Key Laboratory of High Field Laser Physics and CAS Center for Excellence in Ultra-intense Laser Science， Shanghai Institute of Optics and Fine Mechanics， Chinese Academy of Sciences， Shanghai 201800， China State Key Laboratory of High Field Laser Physics and CAS Center for Excellence in Ultra-intense Laser Science， Shanghai Institute of Optics and Fine Mechanics， Chinese Academy of Sciences， Shanghai 201800， China Perovskite materials and devices have obtained great progress due to their significant optoelectronic properties. Especially， quasi-two-dimensional（2D） halide perovskites have shown promising potential in optoelectronic devices due to their large exciton binding energy， strong exciton-photon coupling and enhanced stability. Moreover， the naturally quantum-well structure of 2D perovskite allows exciton energy transfer from the small- n phase to large- n phase， promoting exciton utilization and population inversion to achieve lasing as optical gain media. Herein， we will introduce the crystal structure and advanced optical properties of quasi-2D perovskite at first， and then summarize several strategies about regulating crystal orientation of quasi-2D perovskite. Finally， we will review the development of quasi-2D perovskite based micro- and nanolaser， and present a summary and prospect for quasi-2D perovskite materials and laser devices in the future. 近年来，钙钛矿材料及器件由于其优异的光电特性取得了巨大的研究进展。特别是准二维卤化物钙钛矿材料，因其具有激子结合能大、激子‐光子强耦合和稳定性好等优点，在光电器件领域显示出很大的应用潜力。此外，准二维钙钛矿中自发形成的量子阱结构允许激子能量从小 n 相转移到大 n 相，能够有效促进激子利用率和粒子数反转，这使得准二维钙钛矿材料能够成为激光器中的光学增益介质。本文首先介绍了准二维钙钛矿的晶体结构和优异的光学性能，进而总结了调节准二维钙钛矿晶相结构的几种策略。最后，回顾了准二维钙钛矿微纳激光器的发展，并对准二维钙钛矿材料和激光器件的研究进行了总结和展望。 准二维钙钛矿 晶相调控 增益介质 激光器 quasi-2D perovskite crystal orientation gain medium laser 1　Introduction 1 Perovskites have attracted considerable attention due to their high photoluminescence quantum yield（PLQY）, large light absorption coefficient, superior carrier mobility and long carrier diffusion length, which have been studied widely in the optoelectronic application such as solar cell, light-emitting diode（LED）, laser and photodetector [ 1 1 - 12 12 1-12 ] . Even though the most widely studied perovskite structure at present is the three-dimensional（3D） perovskite [ 13 13 ] , the quasi-two-dimensional（quasi-2D） perovskites have emerged as rising star candidates in recent years due to their enlarged exciton binding energy, strengthened exciton-photon coupling and enhanced stability as compared with the 3D counterparts. These improved properties of quasi-2D perovskites can be assigned to the introduction of organic cations, which can not only improve the stability of perovskite but also accelerate the exciton radiation recombination process [ 14 14 - 19 19 14-19 ] . In the naturally layered quantum-well structure of quasi-2D perovskite, the exciton energy will transfer from small- n layer to large- n layer, promoting radiation recombination [ 20 20 ] . Currently, quasi-2D perovskite based LED has acquired rapid progress, especially the external quantum efficiency（EQE） of green LED has exceeded 22% [ 21 21 ] . Due to naturally quantum-well structure, large exciton binding energy and strong exciton-photon coupling, quasi-2D perovskite has shown potential promising as optical gain media for nanolaser [ 22 22 ] . Moreover, quasi-2D perovskite films have more facile fabrication process and adaption to substrates than 3D perovskite structure, which are much favorable for the integration with various cavity [ 23 23 - 25 25 23-25 ] . In recent years, micro- and nanolaser devices based on quasi-2D perovskite have been realized with various cavities, including single-crystal, whispering gallery mode（WGM）, Fabry‑Perot（F-P） cavities, distributed feedback（DFB）, distributed Bragg reflector（DBR） and photonic crystal structures [ 26 26 - 28 28 26-28 ] . Especially, deep subwavelength quasi-2D perovskite single-mode nanolaser with simple structure has been obtained successfully [ 29 29 ] . In addition, room temperature stabilized continuous-wave（CW） lasing also has been realized in quasi-2D perovskite [ 25 25 , 30 30 - 35 35 30-35 ] . All these exciting micro- and nanolasers based on quasi-2D perovskites demonstrate their great potential for the development of electrically pumped lasers. In this review, we mainly review and discuss the structure, optical properties, the crystallization orientation and the micro/nanolaser application of quasi-2D perovskite. Firstly, we introduce the structural classification of quasi-2D perovskite according to different crystalline phases and organic cation. Based on unique quantum-well structure, quasi-2D perovskite shows advanced optical properties and better stability. Then the strategies of regulating crystal orientation, which include additive, polymer and process engineering methods, are summarized. We mainly review recent progress of quasi-2D perovskite as gain media for nanolasers, including single-crystals, perovskite films and nanolaser arrays. Finally, we present a summary and outlook for quasi-2D perovskite materials and nanolaser in the future. 2　Structure and Properties 1 2.1　Structure 2 The standard 3D perovskites have an ABX 3 structure, where the A -site represents monovalent cation like Cs, MA or FA, B -site ions are generally metal elements like Pb, Sn and X -site ions represent halide elements such as Cl, Br, and I [ 36 36 ] . In this general structure, six X -site ions coordinated to a B -sites ion form a [ BX 6 ] octahedra, and A -site ion is surrounded by these corner-sharing inorganic octahedra [ 37 37 ] . The properties of the perovskite can be adjusted easily by replacing A , B , and X sites ions. When Goldschmidt tolerance factor（ t ） is between 0.8 and 1.0, a standard 3D perovskite structure can be formed stably [ 38 38 ] . The structure of quasi-2D perovskite can be obtained by cutting along the < 100 > , < 110 > , and < 111 > plane of 3D perovskite and adding alkylammonium cation, leading to three kinds of quasi-2D perovskite with different orientations（ Fig.1 Fig.1 ） [ 36 36 ] . The general formula of < 100 > -oriented quasi-2D perovskites（ Fig.1 Fig.1 （a）） is A ' 2 A n -1 B n X 3 n +1 , where A ’ is monovalent organic spacer cation, A, B, X are the corresponding ions in 3D perovskite and n is the number of inorganic layers. < 100 > -oriented quasi-2D perovs‐kite is favorable for continuous growth of inorganic plate, which is the most commonly studied quasi-2D perovskite [ 39 39 ] . The general formula A ' 2 A n B n X 3 n +2 （ n > 1） belongs to < 110 > -oriented quasi-2D perovskite （ Fig.1 Fig.1 （b））, which is found to be ideal candidate for solid-state lighting material because of its broadband white-light emission at room temperature, mainly being caused by self-trapped excitons and lattice efects [ 40 40 ] . But it is difficult to modulate the thickness of inorganic layers accurately for stable < 110 > crystalline structure [ 41 41 ] . < 111 > -oriented quasi-2D perovskite （ Fig.1 Fig.1 （c）） has the general formula A ' 2 A n -1 ‐ B n X 3 n +3 , in which the B -site cation is usually Bi or Sb [ 42 42 ] . This class of perovskite is one of ideal substitutes for lead-free perovskites, but with poor phase stability and excessive electron hole effective mass, resulting in lack of use for solar cell [ 43 43 - 44 44 43-44 ] .Considering that < 100 > -oriented class is the mostly studied quasi-2D perovskites, our review mainly focuses on this class of quasi-2D perovskites. By the alternation of organic spacer cations, < 100 > -oriented quasi-2D perovskite structure can be further divided into Ruddlesden-Popper（RP）, Dion-Jacobson（DJ）, and alternating cations in the interlayer space（ACI） structure（ Fig.2 Fig.2 ） [ 45 45 ] . The RP composition has a general formula A ' 2 A n -1 B n X 3 n +1 , where A ’ is generally monovalent organic cation [ 46 46 ] . The inorganic layer in quasi-2D RP perovskite is separated by alkyl chains or aryl ammonium cations which are connected by relatively weak van der Waals force（ Fig.2 Fig.2 （a）） [ 47 47 ] . Paritmongkol et al . prepared quasi-2D RP perovskite （BA） 2 MA 3 Pb 4 I 13 and demonstrated a （1/2, 1/2） displacement between adjacent inorganic layers [ 48 48 ] . Because only part of the adjacent organic spacer cations overlap, quasi-2D RP perovskite has a long interlayer distance, resulting in no interaction between inorganic layers [ 46 46 ] . The general formula of quasi-2D DJ perovskite is A ’ A n -1 B n X 3 n +1 , where A ’ is bivalent organic spacer cation with two amino groups. Compared to RP perovskite, the inorganic layers are connected by strong hydrogen bond interaction between the organic and inorganic layers, leading to a relatively smaller interlayer space （ Fig. 2 Fig. 2 （b）） [ 49 49 ] . In 2018, Mao et al . firstly fabricated homologous quasi-2D DJ perovskite‐（3AMP）（MA） 3 Pb 4 I 13 , demonstrating that the inorganic layers are perfectly stacked together without displacement in the crystal plane [ 50 50 ] . The quasi-2D ACI-phase perovskite with formula A ’ A n B n X 3 n +1 was proposed in recent years. The monovalent spacer cations A ’ and A -site ions are arranged alternately in the organic layer, resulting in a （1/2, 0） displacement between inorganic layers （ Fig. 2 Fig. 2 （c）） [ 51 51 ] . In 2017, Soe et al . prepared quasi-2D ACI perovskites （C（NH 2 ） 3 ）-（CH 3 NH 3 ） n Pb n ‐I 3 n +1 , which demonstrated smaller band gap compared to RP and DJ structure due to its lower interlayers distance [ 52 52 ] . Up to now, guanidinium（GA） is the only reported A ’ cation in quasi-2D ACI structure [ 51 51 - 52 52 51-52 ] . 2.2　Optical Properties 2 Quasi-2D perovskite structure has many advantages compared to traditional 3D perovskites due to their alternately arranged organic/inorganic layers structure. They can limit charge carriers to quasi-2D range and form a multiple quantum well naturally [ 53 53 ] . On the other hand, the huge dielectric difference between organic and inorganic layers could influence the electrostatic force in the electron-hole pairs, which could significantly enhance the electron-hole binding energy（ Fig.3 Fig.3 （a）） [ 54 54 ] . The various possibilities based on multiple-quantum-well structures make quasi-2D perovskite an interesting material system for room temperature photoelectric and fundamental physics applications [ 55 55 ] . In quasi-2D perovskite, the influence generated by confinement effect from quantum-well structure is the variation of bandgap [ 45 45 ] . The total bandgap energy in quasi-2D RP perovskite consists of two parts: the energy determined by 3D perovskite and the extra part that caused by quantization energy of electron and hole [ 59 59 ] . Besides traditional method of alternating A, B and X cations in 3D perovskites, the bandgap of quasi-2D perovskites can be also adjusted by controlling n value. Zibouche et al . simulated the band alignment between 3D perovskites（MAPbI 3 , FAPbI 3 , MASnI 3 , and FASnI 3 ） and their corresponding quasi-2D perovskites with different n values using density functional theory techniques, as shown in Fig.3 Fig.3 （b） and （c） [ 57 57 ] . They demonstrated the bandgap of MA⁃PbI 3 gradually decreases 2.41 eV to 1.50 eV with n value increasing from 1 to ∞. Wang et al. used the self-assembly BA + precursor cation at the water-air interface as a soft template for inch-scale quasi-2D perovskite single crystal membranes BA 2 MA n -1 Pb n ⁃ I 3 n +1 （ n =1, 2, 3, 4, and ∞） [ 58 58 ] . They demonstrated that the structural, optical and electrical properties of BA 2 MA n -1 Pb n I 3 n +1 are mainly related with quantum well thickness, which can be determined by n values. As shown in the UV-Vis and PL spectra （ Fig.3 Fig.3 （d） and （e）） of quasi-2D perovskites BA 2 MA n -1 Pb n I 3 n +1 with different n values, the bandgap shifts from 1.5 eV to 2.3 eV with n increasing from 1 to ∞. Quasi-2D perovskite tends to spontaneously aggregate in the process of synthesis leading to a quasi-2D perovskite system with different n -values, which is favorable for the energy transfer among mixed phases. Hence, the photoexcitation could be focused on high n value domain, facilitating the formation of population inversion, therefore is fascinating for optical gain medium [ 58 58 ] . In 2017, Liu et al . observed the consecutive photoinduced charge carriers transfer in quasi-2D perovskite （BA） 2 （MA） n -1 Pb n I 3 n +1 films with mixture of multiple perovskite phases with n =2, 3, 4 and ≈∞ [ 60 60 ] . They found that the mixed phases naturally aligned in the order of n along the direction perpendicular to the substrate. Consecutive photoinduced electron transfer from small- n to large- n phases and hole transfer in the opposite direction were observed, which facilitated the charge contraction, and thus lay the foundation for their novel applications in optical gain medium. The room-temperature ASE from quasi-2D perovskites was firstly observed from （NMA） 2 （FA）Pb 2 Br 1 I 6 by Li et al . in 2018, with gain coefficients as high as > 300 cm -1 （ Fig.3 Fig.3 （f） and （g）） [ 61 61 ] . The （NMA） 2 （FA）Pb 2 Br 1 I 6 -based perovskite thin films had different n -values, allowing rapid and efficient energy funneling from higher energy-bandgap quantum-wells（low n value domain） to lower energy-bandgap quantum-wells（high n value domain） and achieving room-temperature ASE with low threshold （（19±2） µJ·cm -2 ） and high gain coefficient. Moreover, the ASE stability at ambient conditions also shows better performance than 3D perovskite thin films. Zhang et al . also observed room-temperature ASE and lasing from mixed n value phases in quasi-2D perovskites thin film of （BA） 2 ‐（MA） n -1 Pb n Br 3 n +1 . They demonstrated an ultrafast energy transfer from low n value domain to high n value domain, concentrating photoexcitation at the lowest bandgap quantum well（ n ≈∞）and establishing the population inversion for stimulated emission [ 62 62 ] . Their results showed no ASE in small n values 1~3 domains, while n =6 perovskite thin film exhibited the best ASE performance. For semiconductor materials, excitons play an important role in charge transport and optical properties. Excitons of perovskite belong to the Vanier exciton model and are usually observed at low temperatures [ 63 63 ] . When the thermal energy is greater than the binding energy, the excitons rapidly ionize [ 64 64 ] . Due to thin and deep quantum wells of quasi-2D perovskite, the spatial confinement halves the Bohr radius and quadruples the exciton binding energy compared to 3D perovskites, therefore, excitons of quasi-2D perovskite can be observed at room temperature [ 58 58 ] . With the decrease of n value, the binding energy of excitons gradually increases, which is directly related to the changes of quantum well and dielectric constant. Blancon et al . estimated the exciton binding energies as a function of n [ 63 63 ] . The exciton binding energy of BA 2 MA n -1 Pb n I 3 n +1 crystal increased from 220 meV to 380 meV with the decrease of n value （ n =1~5）. The exciton effects can accelerate radiative recombination, leading to a higher photoluminescent quantum yield（PLQY > 80%） [ 14 14 , 16 16 ] . Due to its high in-plane anisotropy and excellent optoelectronic properties, quasi-2D perovskite is considered to perform a greater optical anisotropy than 3D perovskite [ 65 65 ] . Chen et al . fabricated 2D [CH‐（NH 2 ） 2 ][C（NH2） 3 ]PbI 4 crystal and reported its large optical anisotropy [ 66 66 ] . Without specially designing the crystal morphology, a large photoresponse linear dichroic ratio up to 2 and a PL linear dichroic ratio of 4.7 were found in the quasi-2D perovskite, which are equivalent or even higher than those perovskite structure with specially designed shape. This property makes quasi-2D perovskite an ideal candidate for polarization devices. 2.3　Stability 2 Although 3D perovskite exhibits excellent photoelectric properties when used as laser gain medium, its poor stability hindered its further application. In general, quasi-2D perovskites exhibit significantly enhanced stability as compared with the 3D counterpart, due to their hydrophobicity of organic groups and stronger interlay interaction [ 46 46 - 47 47 46-47 , 49 49 , 67 67 - 70 70 67-70 ] . The organic spacer cations act as a barrier on the surface of perovskite film, preventing perovskite structure from direct contact of moisture and diffusion of water（ Fig.4 Fig.4 （a）） [ 35 35 ] . Spanopoulos et al . proved quasi-2D RP perovskite performed better environmental stability by preparing a series of quasi-2D perovskites with different organic spacer cations [butylamine（BA）, pentylamine（PA） and hexylamine（HA）] [ 67 67 ] . They demonstrated that the hydrophobicity increased with the length of the organic spacer molecules increasing（ Fig.4 Fig.4 （b）） [ 67 67 ] . Moreover, overlooking the little effect on the optical properties, increasing the length of organic spacer can improve the air, heat, and light stability of quasi-2D perovskite. Finally, the obtained （PA） 2 （MA） 2 Pb n I 7 films on crystalline Si can be air stable for more than 450 d（relative humidity=（20%-80%）±5%）. Moreover, the organic layers in quasi-2D perovskite can act as a barrier in the structure, which can prevent inorganic cations from migrating （ Fig.4 Fig.4 （c）） [ 73 73 - 74 74 73-74 ] . Therefore, quasi-2D perovskites can be used to modify the surface of 3D bulk perovskite and enhance device performance. Han 　 et al . designed surface-quasi-2D （（PEA） 2 PbI 4 ）/bulk-3D（FA 0.98 Cs 0.02 PbI 3 ） hetero-phased perovskite nanograins for long-term-stable LEDs [ 72 72 ] . They found that quasi-2D surface functionalized perovskite demonstrated not only significantly reduced trap density and ion migration, but also rapid radiative recombination due to its spatially and potentially confined charge carriers. As a result, the hetero-phased perovskite LEDs showed substantial improvement in operational lifetime compared to conventional pure 3D or quasi-2D counterparts（ Fig.4 Fig.4 （d）） [ 72 72 ] . On the other hand, quasi-2D perovskites have a better thermodynamic stability compared to traditional 3D perovskites due to the alternately arrangement of organic/inorganic layers and stronger interaction among organic spacer cations and BX 6 octahedra [ 75 75 ] . Compared to RP ones, quasi-2D DJ-phase perovskites usually have better stability, since the strong hydrogen bond in DJ perovskite is more stable than the van der Waals interaction in RP perovskite [ 49 49 ] . Moreover, the closer interlayer distance in DJ perovskite is favorable for the interaction of adjacent inorganic layers, which performs enhanced optical properties and thermodynamics stability. Zhao et al . prepared quasi-2D DJ perovskite（FPP）PbI 4 thin films, which exhibits phase stability with the temperature up to 230 ℃. In contrast, the RP perovskite （PMA） 2 PbI 4 almost degraded completely at 157 ℃ [ 76 76 ] . Moreover, the photostability is also enhanced in quasi-2D perovskites, since the hydrophobic organic spacer effectively passivates the perovskite crystal lattice against moisture and oxygen, which reduces the formation of reactive oxygen species under light [ 77 77 ] . 3　Crystallization Regulation 1 Quasi-2D perovskites show excellent photoelectric property due to their special crystal structure and have been widely used in the field of optoelectronic devices. The crystal phase structures affect their photoelectric properties, since the crystallization orientation of quasi-2D perovskite films could influence the charge transfer effectively [ 78 78 ] . The accurate regulation of crystal orientation can effectively promote photo-generated carrier transport and induce radiative recombination. Therefore, controlling the crystal orientation of quasi-2D perovskite films is crucial for manufacturing efficient devices [ 78 78 - 79 79 78-79 ] . As for semiconductor lasers, the gain property of gain media is critical for the performance, which has great correlation with the crystallization quality of perovskite crystals and films [ 80 80 ] . The accumulation of heat and defects of gain media mainly hinder the performance of optical-pump laser. Therefore, several strategies can be used to enhance structural stability and suppress the formation of photoinduced defects of quasi-2D perovskite, such as compositional engineering or external additives. 3.1　Solvent Engineering 2 Quasi-2D perovskite films are mainly fabricated through simple solution process, in which the polarity, viscosity of solvent and the coordination will affect the crystallization of quasi-2D perovskite. Especially, the crystallization rate of the perovskite phase can be controlled by using specific solvent. Dimethyl sulfoxide（DMSO） and N, N-dimethylformamide（DMF） are commonly used as solvent for the crystallization of perovskite [ 81 81 - 82 82 81-82 ] . When DMF is used as solvent for perovskite precursor only, DMF can be evaporated rapidly at the gas-liquid interface, which can cause random-orientated perovskite grains in the inner layer of perovskite films（Case 1 in Fig.5 Fig.5 （a）） [ 83 83 ] . In comparation, when the mixture of DMF and DMSO are used as solvent, the nucleation process will be slowed down due to the formation of intermediate from DMSO and perovskite precursor and then the crystal grows perpendicular to the substrate （Case 2 in Fig.5 Fig.5 （a））. In 2018, Hamill et al . investigated the role of different solvent（DMSO, DMPU, DMAC, NMP, GBL, EC, PC, et al. ） in the precursors containing Pb 2+ . They introduce Gutmann’s donor number（ D N ） to represent the coordination ability of solvent with Pb 2+[84] . Low D N value solvent has little effect on Pb 2+ , which is conducive to the combination of Pb 2+ and I - . By contrast, those solvents with high D N could coordinate more strongly with Pb 2+ , in turn inhibiting I - coordination and stalling perovskite crystallization. Varying the concentration of high D N additives in precursor solutions could tunes the strength of lead solvent interactions effectively, allowing finer control over the crystallization and morphology of perovskite active layers（ Fig.5 Fig.5 （b））. In addition, ionic liquid can be also used as solvent to regulate the crystallization of quasi-2D perovskite [ 85 85 ] . The physical properties of ionic liquid, such as high conductivity and low viscosity can be adjusted by varying the combination of cations and anions. In 2016, Yang et al . firstly reported the application of ionic liquid （1-benzyl-3-meth-ylimidazolium chloride） in perovskite solar cells based on quasi-2D perovskite （HC（NH 2 ） 2 PbI 3 ） 0.85 （CH 3 NH 3 -PbBr 3 ） 0.15 . They demonstrated that ionic liquid can effectively promote the reduction of the electron trap-state density at perovskite surface. Finally they fabricated quasi-2D perovskite-based solar cell with improved power conversion efficiency（PCE） of 16.09% [ 86 86 ] . In 2021, Peng et al . treated Pb-based perovskite thin films with ionic liquid 1-butyl- 3-methylimidazolium tetrafluoroborate（BMIMBF 4 ）, which can effectively passivate defect due to the spontaneous distribution of ions on film top surface and the crystal surface of the polycrystalline perovskite（ Fig.5 Fig.5 （c）） [ 87 87 ] . Then, they obtained highly efficient LED with EQE of 22.9%. 3.2　Additives Engineering 2 Additive can be usually used to improve the quality of perovskite film and the performance of device through the control of crystal orientation and surface modification [ 89 89 ] . In 2020, Li et al . adopted CH 3 NH 3 Cl（MACl） as an additive to obtain a （PTA） 2 ‐（MA） 3 Pb 4 I 13 film with highly oriented crystal structure and uniform surface morphology [ 90 90 ] , which enable superior charge transfer capability and low-density defect states. The highly oriented crystal structure can be attributed to the interaction between Cl - of MACl additive and Pb 2+ . Finally, the optimized device showed PCE of 11.53% and enhanced stability. Then Huang et al . also used MACl as additive to modifying quasi-2D RP perovskite （PEA） 2 （MA） 4 Pb 5 I 16 films through facile one-step process [ 91 91 ] . They demonstrated that the MACl additive can form an intermediate phase to facilitate the vertical alignment of quasi-2D RP perovskite film on the substrate. Finally, they improved the PCE of solar cell from 0.66% to 9.7% by introducing MACl as additive. Besides, ammonium chloride（NH 4 Cl） can also be used as effect additive for quasi-2D perovskite precursor solution to regulate the crystal orientation [ 82 82 ] . In 2018, Fu et al . adopted NH 4 Cl and NH 4 SCN as additive to obtain quasi-2D perovskite （PEA） 2 （MA） 4 Pb 5 I 16 film with better crystallinity and preferential orientation [ 92 92 ] . Both additives can improve the crystallinity of perovskite film, but compared with NH 4 Cl, NH 4 SCN is more effective. However, tiny pinholes appeared in the film with only NH 4 SCN as additive, compact and uniform films are obtained with only NH 4 Cl or both additives. Moreover, the addition of NH 4 Cl increases the concentration of Cl - at the perovskite interface in solar cell, which can passivate the electron trap and improves the external quantum effect of electroluminescence. Then they fabricated （PEA） 2 （MA） 4 Pb 5 I 16 -based solar cell with PCE of 14.1%. In 2020, Yuan et al . used NH 4 Cl additive to inhibit PbI 2 -DMF-contained solvate phases（PDS） precipitation for the first time, thus achieved the regulation of perovskite crystal nucleus density in solution [ 93 93 ] . NH 4 Cl additive can change the growth behavior of quasi-2D perovskite from top to bottom into the main growth mechanism, and increase the grain size by inhibiting nucleation. Vertically oriented grains obtained at room temperature solution can overcome the problem of poor conductivity of quasi-2D perovskite layers and significantly improve the energy conversion efficiency of solar cells [ 93 93 ] . There have been many polymer additives can be used to regulate the crystallization process of quasi-2D perovskite films, which generally contain hydroxyl, carboxyl, carbonyl and other hydrophilic groups, coordinating with Pb 2+ in perovskite. In 2021, Liu et al . used 18-crown-6 and poly （ethylene glycol） methyl ether acrylate （MPEG-MAA） as additives to obtain quasi-2D perovskite PEABr∶CsPbBr 3 film [ 88 88 ] . They found that the C—O—C bond in the additives can reduced the self-polymerization of organic ligands, enabling higher-quality nanocrystals（ Fig.5 Fig.5 （d））. Then, they fabricated a highly efficient green light LED with a maximum EQE of 28.1%. In 2022, Cao et al . used （biodegradability） poly （butylene adipate-coterephthalate） polymer（PBAT） as additive to fabricate CsMAFA-based perovskite film with high quality [ 78 78 ] . They proved that carbonyl groups and benzene rings of PBAT polymer can passivate the undercoordinated Pb 2+ and defects of perovskite, which can regulate the crystallization of perovskite films. They obtained a highly efficient perovskite solar cell with PCE of 22.07%. 3.3　Process Engineering 2 In the crystallization process of quasi-2D perovskite films, temperature, humidity and rotation speed can affect the quality. In 2016, Tsai et al . reported a hot-coating process for the fabrication of high-quality （BA） 2 （MA） n -1 Pb n I 3 n +1 perovskite film [ 94 94 ] . Compared with the spin coated film at room temperature, the morphology of the quasi-2D perovskite film prepared by hot-casting is superior and the film quality is improved. The PCE of obtained the solar cells reaches 12.52% by using hot-casting method, and the stability of the device is greatly improved. The unpackaged devices can maintain an efficiency of 65% or more in standard （AM1.5G） illumination for more than 2 250. In 2019, Yang et al . found that CsPbIBr 2 film has better growth on In 2 S 3 films compared with TiO 2 films, which can be attribute to the reduction of Gibbs free energy on the In 2 S 3 film surface, promoting the formation of perovskite film with smooth, pinhole-free and high crystallinity [ 95 95 ] . And they obtained a high efficiency solar cell with a PCE of 5.59% with reduced hysteresis. In 2021, Luo et al . realized the directional growth of FA 0.75 MA 0.25 ‐PbI 3 perovskite film via quasi-2D-seed （（BDA）PbI 4 ） induction [ 96 96 ] . In this seed induction method, the 2D seed solution is spin-coated on the substrate, which can act as templates for the growth of 3D perovskite with the desired facet orientation. Then the precursor containing 3D perovskite is spin-coated on the first film. The 2D seeds can be transformed into the grain boundary after completing the orientation- induced growth. They found that this process can control crystallization and facilitate the epitaxial growth of 3D perovskite, resulting in a film with the desired growth direction. The high-performance perovskite based solar cell was fabricated by using seed-induced method with PCE of 23.95% and high fill factor of 0.847. 4　Perovskite Lasers 1 Organic-inorganic hybrid quasi-2D perovskites have recently attracted great attention in optical and optoelectronic applications due to their inherent natural quantum-well structure [ 25 25 ] . Thin films of quasi-2D perovskites typically contain a mixture of domains with different layers. Within such inhomogeneous domain distribution, it is assumed that the energy rapidly funnels from the high-bandgap domains to the low-bandgap domains and finally emits radiatively, resulting in rapid charge-carrier localization and increased carrier concentration in acceptors [ 97 97 ] . This process improves the rate of radiative recombination and facilitates the buildup of population inversion. Therefore, quasi-2D perovskites are promising gain media for laser applications [ 98 98 ] . 4.1　Perovskite Single‑crystal Lasers 2 Quasi-2D perovskite single crystals have advantages of rectangular boundary, low defect density and pure phase, which can contribute to the realization of quasi-2D perovskite laser. In 2018, Raghavan et al . prepared high-quality RP quasi-2D perovskite （BA） 2 （MA） n -1 Pb n I 3 n +1 （ n =1, 2, 3） single crystals with millimeter size through slow evaporation at constant temperature（SECT） solution-growth process [ 68 68 ] . The single crystal with pyramidal structure has good crystallinity, phase purity and spectral uniformity（ Fig.6 Fig.6 （a））. Then they obtained tunable laser with low threshold at room temperature. The laser thresholds are 2.85 μJ/cm 2 （ n =1）, 3.02 μJ/cm 2 （ n =2） and 3.21 μJ/cm 2 （ n =3）（ Fig.6 Fig.6 （b）） respectively. Then in 2020, this group adopted SECT method to fabricate quasi-2D perovskite FA-（N-MPDA）PbBr 4 （N-MPDA=N-1-methylpropane-1,3-diammonium） single crystal microrods（ Fig.6 Fig.6 （c）） [ 99 99 ] . They observed high-quality, low threshold（~0.5 μJ/cm 2 ） random lasing in microrods at room temperature, which can retain after 2 h under continuous lasing irradiation（ Fig.6 Fig.6 （d））. In 2019, Liang et al . investigated the mechanism of lasing and loss in quasi-2D perovskite （BA）（MA） n -1 Pb n I 3 n +1 thin microflakes and discovered the effect of Auger recombination and exciton phonon coupling on lasing [ 100 100 ] . They proved that multicolor lasing can be achieved from the large- n RPPs（ n ≥3） in the spectral range of 620-680 nm（ Fig.6 Fig.6 （e）-（g））. With decreasing n , the lasing threshold increases significantly and the characteristic temperature decreases as 49, 25, 20 K for n =5, 4, 3, respectively（ Fig.6 Fig.6 （h））. Most recently, Zhang et al . fabricated high-quality quasi-2D perovskite single crystals with mechanically exfoliated flakes with high crystallinity. Then they embedded PEA 2 PbI 4 in a vertical microcavity to realized single-mode continuous-wave laser with low threshold 5.7 W/cm 2 at room temperature [ 101 101 ] . 4.2　Quasi‑2D Perovskite Film Lasers 2 Quasi-2D perovskite films are not only simple in preparation, but also have high quality, good surface morphology and low defect density, which have great potential as gain medium in micro- and nanolaser. In 2018, Edward et al .prepared （C 12 H 25 NH 3 ） 2 PbI 4 perovskite film, which can be used as optical medium in an optical microcavity [ 102 102 ] . Then, they observed biexciton lasing in a vertical cavity（comprising a distributed Bragg reflector and a metal mirror） above 125 K, with a threshold peak excitation density of 5.6 × 10 18 cm -3 . In 2019, Matthew et al . investigated the feasibility of quasi-2D perovskite for electrically pumped lasers. They obtained optically driven DFB lasers from low-dimensional NMA-based perovskite with a FWHM of less than 1 nm. They stated that the current density probably needs to reach 4-10 kA/cm 2 to achieve the emission of electrically pumped laser [ 23 23 ] . In 2022, Zhong's group obtained single-mode vertical-cavity lasing from CsPbC l1.5 Br 1.5 -based quasi-2D perovskites between two DBR mirrors with low threshold of 9.2 μJ/cm 2 （ Fig. 7 Fig. 7 （a）） [ 24 24 ] . They found the perovskite film using 2,2-diphenylethylammonium bromide（DPEABr） as ligand has a large- n -phase narrow distribution, which enable enough exciton energy transfer and inhabit Auger recombination（ Fig.7 Fig.7 （b））. In 2021, Liu et al . proposed an ultra-simple “sandwich” cavity structure based on the quasi-2D perovskite thin film to enhance the interaction between light and matter at the nanoscale（ Fig.7 Fig.7 （c）） [ 29 29 ] . The room temperature single-mode picosecond laser has been successfully achieved with low threshold（~10 μJ/cm 2 ）, narrow line width（~0.3 nm） and high degree of polarization（~81%） in the deep subwavelength scale 40 nm perovskite film and 10 nm glue layer（ Fig.7 Fig.7 （d））. The laser device overcame the diffraction limit without the help of metal plasma, which was the smallest size of all-medium semiconductor laser. This realization of deep subwavelength scale quasi-2D perovskite laser could provide a strong driving force for electrically pumped perovskite laser devices with high gain and effective electron-hole recombination to balance the trade-off between carrier injection and transmission distance in subwavelength scale [ 29 29 ] . In 2022, Li et al . prepared CsPbBr 3 （BABr） x /CsPbBr 3 perovskite planar heterojunction structure as gain medium of laser [ 103 103 ] . Importantly, this structure can facilitate the transfer of excited states from the broadband quasi-2D perovskite to narrow-band 3D perovskite. Then they obtained vertical cavity surface-emitting laser based on planar heterojunction structure with low threshold of （46±15） μJ/cm 2 . In addition, there have been several reports about perovskite-based CW lasers [ 104 104 - 106 106 104-106 ] . In 2019, Philipp et al . realized CW ASE from phase-stabilized perovskites（Cs 0.1 （MA 0.17 FA 0.83 ） 0.9 Pb 0.84 （I 0.84 Br 0.16 ） 2.68 ） at a temperature up to 120 K [ 105 105 ] . The threshold of obtained CW ASE is 387 W/cm 2 at 80 K. This phase-stabilized perovskite retains the room-temperature phase at low temperature and has the potential to support CW laser at higher temperature. In 2020, Qin et al . investigated the effect of singlet and triplet states on particle number inversion in FAPbBr 3 -based quasi-2D perovskite containing different cations and prepared a stable green quasi-2D laser with CW laser pump [ 107 107 ] . They prepared PEABr-based perovskite（P2F8） films with high triplet energy and NMABr-based perovskite（N2F8） films（ n =8） with low triplet energy respectively（ Fig.7 Fig.7 （e））. They found that singlet-triplet exciton annihilation is the main intrinsic mechanism causing lasing loss. Then, they fabricated a DFB laser by rotating quasi-2D perovskite film onto a substrate with 2D grating（ Fig.7 Fig.7 （f））. Finally, they successfully obtained CW laser based on P2F8 and N2F8 with threshold of 59 W/cm 2 and 45 W/cm 2 , respectively（ Fig.7 Fig.7 （g））. In 2021, Lu et al . demonstrated stable pure blue emission ~471 nm under CW laser irradiation with high power density of 81 W/cm 2 from mixed-Br/Cl Cs-based quasi-2D perovskite films by a facile vapor anion exchange（VAE） process [ 101 101 ] . The advantage of VAE method is that Cl can be introduced into the lattice without destroying the morphology, overcoming low solubility of Cl in the precursor solution. In addition, changing the VAE processing time can effectively control the bandgap of perovskite film, resulting in tunable ASE changing from 537 nm to 475 nm. 4.3　Quasi‐2D Perovskite Lasers Array 2 In 2018, Zhang et al . prepared quasi-2D RP perovskite BA 2 FA n -1 Pb n Br 3 n +1 film with n =3, and achieved ASE at room temperature. Finally they fabricated nanowire laser array with high quality （ Q ） factor（~1 800） and low lasing threshold of ~27-31 μJ/cm 2 by using polydimethylsiloxane（PDMS） template confined solution-growth method（ Fig.7 Fig.7 （h）） [ 107 107 ] . They indicated that high-energy small- n -value QWs（ n =2, 4, 5） acting as energy antenna captured more energies from the excited light, then an ultrafast energy transfer to low-energy large- n -value QWs（ n > 5）, leads to rapid accumulation of excitons and therefore induces population inversion for the ASE process. Later, they prepared quasi-2D RP perovskite BA 2 MA n -1 Pb n Br 3 n +1 film and achieved ASE from the film with n =6 with low threshold of 13.6 μJ/cm 2[ 62 62 ] . Furthermore, they fabricated microrings whispering-gallery-mode（WGM） laser array based on quasi-2D perovskite with high quality （ Q ） factor of 2 600, as show in Fig.7 Fig.7 （i）. Moreover, they demonstrated different numbers of resonance modes can be obtained on RP perovskite microrings with different diameter（ Fig.7 Fig.7 （j）） [ 62 62 ] . 5　Conclusion and Outlook 1 Layered quasi-2D halide perovskites have been studied widely as an advanced class of semiconductor materials due to their unique optoelectronic properties. In this review, the crystal structure, optical properties and stability of quasi-2D lead halide perovskites are mainly reviewed. Then the recent research progress of crystal growth regulating is introduced and the applications in laser devices are briefly discussed. Compared to traditional 3D perovskites, quasi-2D perovskites have many fascinating properties, such as enhanced stability, flexibility in structure adjustment, and ultra-fast energy transfer process. Therefore, quasi-2D perovskites materials have great potential in the field of optoelectronic devices like high-efficient LED due to their advantages of unique multiple quantum-well structure and high gain coefficient. The charge carriers transfer process in quasi-2D perovskite with different n value phases facilitate the population inversion, which produce possibilities for the realization of low threshold laser. However, multiple n -values phase also has negative effects like multipeak emission and lack of repeatability. Therefore, the accurate control of phase purity is important research direct, which might be supported by the development of new processing methods. In addition, some details about electron properties, such as electron-phonon coupling, symmetry effects, exciton optical physics and their effects remain unclear, which hinder the improvement of quasi-2D perovskite optoelectronic devices. It is well known that the ultimate goal for semiconductor laser is electrical pump lasing, which is the biggest challenge for perovskite micro/nanolaser. There are several issues needed to be resolved tremendously, such as the poor stability, high internal resistance and poor thermal conductance of gain media. As for the device, the excessive leakage current, charge imbalance and Joule heating also can reduce the device performance, hindering the realization of electrical pump lasing. Therefore, to develop perovskite-based electrically pumped lasers, several urgent strategies should be performed including material engineering especially thermal management of gain media, cavity engineering and charge balance of laser device. As the perovskite materials and optoelectronic devices developing rapidly, we believe in the emergence of electrically pumped lasers in the near future. 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WANG Jun,ZHOU Feng-xian,LI Qian,et al.Quasi-2D Lead Halide Perovskites for Micro- and Nanolasers[J].Chinese Journal of Luminescence,2022,43(11):1645-1662. 国家自然科学基金（61875211, 62005296, 62205081, 61925507, 61905264, 92050203, 62105347）； 中国科学院创新交叉团队项目； 上海市科技计划项目（22JC1403200）； 杭州市领军型创新团队项目（TD2020002）； 国科大杭州高等研究院专项（2022ZZ01001，2022ZZ01005）资助项目 Supported by National Natural Science Foundation of China （61875211, 62005296, 62205081, 61925507, 61905264, 92050203, 62105347）； CAS Interdisciplinary Innovation Team；Shanghai Pilot Program for Basic Research（22JC1403200）； Hangzhou Science and Technology Bureau of Zhejiang Provience（TD2020002）； The Research Funds of Hangzhou Institute for Advanced Study, UCAS（2022ZZ01001，2022ZZ01005） 2022-05-05 2022-05-23 2022-11-05 2022-12-08 发光学报 11 43