Amide‐Catalyzed Phase‐Selective Crystallization Reduces Defect Density in Wide‐Bandgap Perovskites

Wide‐bandgap (WBG) formamidinium–cesium (FA‐Cs) lead iodide–bromide mixed perovskites are promising materials for front cells well‐matched with crystalline silicon to form tandem solar cells. They offer avenues to augment the performance of widely deployed commercial solar cells. However, phase instability, high open‐circuit voltage (V_oc) deficit, and large hysteresis limit this otherwise promising technology. Here, by controlling the crystallization of FA‐Cs WBG perovskite with the aid of a formamide cosolvent, light‐induced phase segregation and hysteresis in perovskite solar cells are suppressed. The highly polar solvent additive formamide induces direct formation of the black perovskite phase, bypassing the yellow phases, thereby reducing the density of defects in films. As a result, the optimized WBG perovskite solar cells (PSCs) (E_g ≈ 1.75 eV) exhibit a high V_oc of 1.23 V, reduced hysteresis, and a power conversion efficiency (PCE) of 17.8%. A PCE of 15.2% on 1.1 cm² solar cells, the highest among the reported efficiencies for large‐area PSCs having this bandgap is also demonstrated. These perovskites show excellent phase stability and thermal stability, as well as long‐term air stability. They maintain ≈95% of their initial PCE after 1300 h of storage in dry air without encapsulation.     

A 1300 mm2 Ultrahigh‐Performance Digital Imaging Assembly using High‐Quality Perovskite Single Crystals

By fine‐tuning the crystal nucleation and growth process, a low‐temperature‐gradient crystallization method is developed to fabricate high‐quality perovskite CH₃NH₃PbBr₃ single crystals with high carrier mobility of 81 ± 5 cm² V^?1 s^?1 (>3 times larger than their thin film counterpart), long carrier lifetime of 899 ± 127 ns (>5 times larger than their thin film counterpart), and ultralow trap state density of 6.2 ± 2.7 × 10⁹ cm^?3 (even four orders of magnitude lower than that of single‐crystalline silicon wafers). In fact, they are better than perovskite single crystals reported in prior work: their application in photosensors gives superior detectivity as high as 6 × 10¹³ Jones, ≈10–100 times better than commercial sensors made of silicon and InGaAs. Meanwhile, the response speed is as fast as 40 µs, ≈3 orders of magnitude faster than their thin film devices. A large‐area (≈1300 mm²) imaging assembly composed of a 729‐pixel sensor array is further designed and constructed, showing excellent imaging capability thanks to its superior quality and uniformity. This opens a new possibility to use the high‐quality perovskite single‐crystal‐based devices for more advanced imaging sensors.     

Room‐Temperature Solution‐Synthesized p‐Type Copper(I) Iodide Semiconductors for Transparent Thin‐Film Transistors and Complementary Electronics

Here, room‐temperature solution‐processed inorganic p‐type copper iodide (CuI) thin‐film transistors (TFTs) are reported for the first time. The spin‐coated 5 nm thick CuI film has average hole mobility (µ_FE) of 0.44 cm² V^?1 s^?1 and on/off current ratio of 5 × 10². Furthermore, µ_FE increases to 1.93 cm² V^?1 s^?1 and operating voltage significantly reduces from 60 to 5 V by using a high permittivity ZrO₂ dielectric layer replacing traditional SiO₂. Transparent complementary inverters composed of p‐type CuI and n‐type indium gallium zinc oxide TFTs are demonstrated with clear inverting characteristics and voltage gain over 4. These outcomes provide effective approaches for solution‐processed inorganic p‐type semiconductor inks and related electronics.     

300% Enhancement of Carrier Mobility in Uniaxial‐Oriented Perovskite Films Formed by Topotactic‐Oriented Attachment

Organic–inorganic perovskites with intriguing optical and electrical properties have attracted significant research interests due to their excellent performance in optoelectronic devices. Recent efforts on preparing uniform and large‐grain polycrystalline perovskite films have led to enhanced carrier lifetime up to several microseconds. However, the mobility and trap densities of polycrystalline perovskite films are still significantly behind their single‐crystal counterparts. Here, a facile topotactic‐oriented attachment (TOA) process to grow highly oriented perovskite films, featuring strong uniaxial‐crystallographic texture, micrometer‐grain morphology, high crystallinity, low trap density (≈4 × 10¹⁴ cm^?3), and unprecedented 9 GHz charge‐carrier mobility (71 cm² V^?1 s^?1), is demonstrated. TOA‐perovskite‐based n‐i‐p planar solar cells show minimal discrepancies between stabilized efficiency (19.0%) and reverse‐scan efficiency (19.7%). The TOA process is also applicable for growing other state‐of‐the‐art perovskite alloys, including triple‐cation and mixed‐halide perovskites.     

2D Ca3Sn2S7 Chalcogenide Perovskite: A Graphene‐Like Semiconductor with Direct Bandgap 0.5 eV and Ultrahigh Carrier Mobility 6.7 × 104 cm2 V−1 s−1

Graphene, a star 2D material, has attracted much attention because of its unique properties including linear electronic dispersion, massless carriers, and ultrahigh carrier mobility (10⁴–10⁵ cm² V^?1 s^?1). However, its zero bandgap greatly impedes its application in the semiconductor industry. Opening the zero bandgap has become an unresolved worldwide problem. Here, a novel and stable 2D Ruddlesden–Popper‐type layered chalcogenide perovskite semiconductor Ca₃Sn₂S₇ is found based on first‐principles GW calculations, which exhibits excellent electronic, optical, and transport properties, as well as soft and isotropic mechanical characteristics. Surprisingly, it has a graphene‐like linear electronic dispersion, small carrier effective mass (0.04 m₀), ultrahigh room‐temperature carrier mobility (6.7 × 10⁴ cm² V^?1 s^?1), Fermi velocity (3 × 10⁵ m s^?1), and optical absorption coefficient (10⁵ cm^?1). Particularly, it has a direct quasi‐particle bandgap of 0.5 eV, which realizes the dream of opening the graphene bandgap in a new way. These results guarantee its application in infrared optoelectronic and high‐speed electronic devices.     

The Role of Rubidium in Multiple‐Cation‐Based High‐Efficiency Perovskite Solar Cells

Perovskite solar cells (PSCs) based on cesium (Cs)‐ and rubidium (Rb)‐containing perovskite films show highly reproducible performance; however, a fundamental understanding of these systems is still emerging. Herein, this study has systematically investigated the role of Cs and Rb cations in complete devices by examining the transport and recombination processes using current–voltage characteristics and impedance spectroscopy in the dark. As the credibility of these measurements depends on the performance of devices, this study has chosen two different PSCs, (MAFACs)Pb(IBr)₃ (MA = CH₃NH₃⁺, FA = CH(NH₂)₂⁺) and (MAFACsRb)Pb(IBr)₃, yielding impressive performances of 19.5% and 21.1%, respectively. From detailed studies, this study surmises that the confluence of the low trap‐assisted charge‐carrier recombination, low resistance offered to holes at the perovskite/2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9‐spirobifluorene interface with a low series resistance (R_s), and low capacitance leads to the realization of higher performance when an extra Rb cation is incorporated into the absorber films. This study provides a thorough understanding of the impact of inorganic cations on the properties and performance of highly efficient devices, and also highlights new strategies to fabricate efficient multiple‐cation‐based PSCs.     

Enhancing Performance of Nonfullerene Acceptors via Side‐Chain Conjugation Strategy

A side‐chain conjugation strategy in the design of nonfullerene electron acceptors is proposed, with the design and synthesis of a side‐chain‐conjugated acceptor (ITIC2) based on a 4,8‐bis(5‐(2‐ethylhexyl)thiophen‐2‐yl)benzo[1,2‐b :4,5‐b′ ]di(cyclopenta‐dithiophene) electron‐donating core and 1,1‐dicyanomethylene‐3‐indanone electron‐withdrawing end groups. ITIC2 with the conjugated side chains exhibits an absorption peak at 714 nm, which redshifts 12 nm relative to ITIC1. The absorption extinction coefficient of ITIC2 is 2.7 × 10⁵m ^?1 cm^?1, higher than that of ITIC1 (1.5 × 10⁵m ^?1 cm^?1). ITIC2 exhibits slightly higher highest occupied molecular orbital (HOMO) (?5.43 eV) and lowest unoccupied molecular orbital (LUMO) (?3.80 eV) energy levels relative to ITIC1 (HOMO: ?5.48 eV; LUMO: ?3.84 eV), and higher electron mobility (1.3 × 10^?3 cm² V^?1 s^?1) than that of ITIC1 (9.6 × 10^?4 cm² V^?1 s^?1). The power conversion efficiency of ITIC2‐based organic solar cells is 11.0%, much higher than that of ITIC1‐based control devices (8.54%). Our results demonstrate that side‐chain conjugation can tune energy levels, enhance absorption, and electron mobility, and finally enhance photovoltaic performance of nonfullerene acceptors.     

Self‐Sorting of 10‐µm‐Long Single‐Walled Carbon Nanotubes in Aqueous Solution

Single‐walled carbon nanotubes (SWCNTs) are a class of 1D nanomaterials that exhibit extraordinary electrical and optical properties. However, many of their fundamental studies and practical applications are stymied by sample polydispersity. SWCNTs are synthesized in bulk with broad structural (chirality) and geometrical (length and diameter) distributions; problematically, all known post‐synthetic sorting methods rely on ultrasonication, which cuts SWCNTs into short segments (typically <1 µm). It is demonstrated that ultralong (>10 µm) SWCNTs can be efficiently separated from shorter ones through a solution‐phase “self‐sorting”. It is shown that thin‐film transistors fabricated from long semiconducting SWCNTs exhibit a carrier mobility as high as ≈90 cm² V^?1 s^?1, which is ≈10 times higher than those which use shorter counterparts and well exceeds other known materials such as organic semiconducting polymers (<1 cm² V^?1 s^?1), amorphous silicon (≈1 cm² V^?1 s^?1), and nanocrystalline silicon (≈50 cm² V^?1 s^?1). Mechanistic studies suggest that this self‐sorting is driven by the length‐dependent solution phase behavior of rigid rods. This length sorting technique shows a path to attain long‐sought ultralong, electronically pure carbon nanotube materials through scalable solution processing.     

Enhancing the Performance of Polymer Solar Cells via Core Engineering of NIR‐Absorbing Electron Acceptors

In order to utilize the near‐infrared (NIR) solar photons like silicon‐based solar cells, extensive research efforts have been devoted to the development of organic donor and acceptor materials with strong NIR absorption. However, single‐junction organic solar cells (OSCs) with photoresponse extending into >1000 nm and power conversion efficiency (PCE) >11% have rarely been reported. Herein, three fused‐ring electron acceptors with varying core size are reported. These three molecules exhibit strong absorption from 600 to 1000 nm and high electron mobility (>1 × 10^?3 cm² V^?1 s^?1). It is proposed that core engineering is a promising approach to elevate energy levels, enhance absorption and electron mobility, and finally achieve high device performance. This approach can maximize both short‐circuit current density ( J_SC) and open‐circuit voltage (V_OC) at the same time, differing from the commonly used end group engineering that is generally unable to realize simultaneous enhancement in both V_OC and J_SC. Finally, the single‐junction OSCs based on these acceptors in combination with the widely polymer donor PTB7‐Th yield J_SC as high as 26.00 mA cm^?2 and PCE as high as 12.3%.     

Achieving Large‐Area Planar Perovskite Solar Cells by Introducing an Interfacial Compatibilizer

Despite the recent unprecedented increase in the power conversion efficiencies (PCEs) of small‐area devices (≤0.1 cm²), the PCEs deteriorate drastically for PSCs of larger areas because of the incomplete film coverage caused by the dewetting of the hydrophilic perovskite precursor solutions on the hydrophobic organic charge‐transport layers (CTLs). Here, an innovative method of fabricating scalable PSCs on all types of organic CTLs is reported. By introducing an amphiphilic conjugated polyelectrolyte as an interfacial compatibilizer, fabricating uniform perovskite films on large‐area substrates (18.4 cm²) and PSCs with the total active area of 6 cm² (1 cm² × 6 unit cells) via a single‐turn solution process is successfully demonstrated. All of the unit cells exhibit highly uniform PCEs of 16.1 ± 0.9% (best PCE of 17%), which is the highest value for printable PSCs with a total active area larger than 1 cm².     

Fused Hexacyclic Nonfullerene Acceptor with Strong Near‐Infrared Absorption for Semitransparent Organic Solar Cells with 9.77% Efficiency

A fused hexacyclic electron acceptor, IHIC, based on strong electron‐donating group dithienocyclopentathieno[3,2‐b ]thiophene flanked by strong electron‐withdrawing group 1,1‐dicyanomethylene‐3‐indanone, is designed, synthesized, and applied in semitransparent organic solar cells (ST‐OSCs). IHIC exhibits strong near‐infrared absorption with extinction coefficients of up to 1.6 × 10⁵m ^?1 cm^?1, a narrow optical bandgap of 1.38 eV, and a high electron mobility of 2.4 × 10^?3 cm² V^?1 s^?1. The ST‐OSCs based on blends of a narrow‐bandgap polymer donor PTB7‐Th and narrow‐bandgap IHIC acceptor exhibit a champion power conversion efficiency of 9.77% with an average visible transmittance of 36% and excellent device stability; this efficiency is much higher than any single‐junction and tandem ST‐OSCs reported in the literature.     

N‐Type 2D Organic Single Crystals for High‐Performance Organic Field‐Effect Transistors and Near‐Infrared Phototransistors

Organic field‐effect transistors and near‐infrared (NIR) organic phototransistors (OPTs) have attracted world's attention in many fields in the past decades. In general, the sensitivity, distinguishing the signal from noise, is the key parameter to evaluate the performance of NIR OPTs, which is decided by responsivity and dark current. 2D single crystal films of organic semiconductors (2DCOS) are promising functional materials due to their long‐range order in spite of only few molecular layers. Herein, for the first time, air‐stable 2DCOS of n‐type organic semiconductors (a furan‐thiophene quinoidal compound, TFT‐CN) with strong absorbance around 830 nm, by the facile drop‐casting method on the surface of water are successfully prepared. Almost millimeter‐sized TFT‐CN 2DCOS are obtained and their thickness is below 5 nm. A competitive field‐effect electron mobility (1.36 cm² V^?1 s^?1) and high on/off ratio (up to 10⁸) are obtained in air. Impressively, the ultrasensitive NIR phototransistors operating at the off‐state exhibit a very low dark current of ≈0.3 pA and an ultrahigh detectivity (D*) exceeding 6 × 10¹⁴ Jones because the devices can operate in full depletion at the off‐state, superior to the majority of the reported organic‐based NIR phototransistors.     

FA‐Assistant Iodide Coordination in Organic–Inorganic Wide‐Bandgap Perovskite with Mixed Halides

Mixed‐halide wide‐bandgap perovskites are key components for the development of high‐efficiency tandem structured devices. However, mixed‐halide perovskites usually suffer from phase‐impurity and high defect density issues, where the causes are still unclear. By using in situ photoluminescence (PL) spectroscopy, it is found that in methylammonium (MA⁺)‐based mixed‐halide perovskites, MAPb(I_0.6Br_0.4)₃, the halide composition of the spin‐coated perovskite films is preferentially dominated by the bromide ions (Br^?). Additional thermal energy is required to initiate the insertion of iodide ions (I^?) to achieve the stoichiometric balance. Notably, by incorporating a small amount of formamidinium ions (FA⁺) in the precursor solution, it can effectively facilitate the I^? coordination in the perovskite framework during the spin‐coating and improve the composition homogeneity of the initial small particles. The aggregation of these homogenous small particles is found to be essential to achieve uniform and high‐crystallinity perovskite film with high Br^? content. As a result, high‐quality MA_0.9FA_0.1Pb(I_0.6Br_0.4)₃ perovskite film with a bandgap (E_g) of 1.81 eV is achieved, along with an encouraging power‐conversion‐efficiency of 17.1% and open‐circuit voltage (V_oc) of 1.21 V. This work also demonstrates the in situ PL can provide a direct observation of the dynamic of ion coordination during the perovskite crystallization.     

An All‐Solution‐Based Hybrid CMOS‐Like Quantum Dot/Carbon Nanotube Inverter

The development of low‐cost, flexible electronic devices is subordinated to the advancement in solution‐based and low‐temperature‐processable semiconducting materials, such as colloidal quantum dots (QDs) and single‐walled carbon nanotubes (SWCNTs). Here, excellent compatibility of QDs and SWCNTs as a complementary pair of semiconducting materials for fabrication of high‐performance complementary metal‐oxide‐semiconductor (CMOS)‐like inverters is demonstrated. The n‐type field effect transistors (FETs) based on I^? capped PbS QDs (V _th = 0.2 V, on/off = 10⁵, S _S‐th = 114 mV dec^?1, µ _e = 0.22 cm² V^?1 s^?1) and the p‐type FETs with tailored parameters based on low‐density random network of SWCNTs (V _th = ?0.2 V, on/off > 10⁵, S _S‐th = 63 mV dec^?1, µ _h = 0.04 cm² V^?1 s^?1) are integrated on the same substrate in order to obtain high‐performance hybrid inverters. The inverters operate in the sub‐1 V range (0.9 V) and have high gain (76 V/V), large maximum‐equal‐criteria noise margins (80%), and peak power consumption of 3 nW, in combination with low hysteresis (10 mV).     

Polymer Doping Enables a Two‐Dimensional Electron Gas for High‐Performance Homojunction Oxide Thin‐Film Transistors

High‐performance solution‐processed metal oxide (MO) thin‐film transistors (TFTs) are realized by fabricating a homojunction of indium oxide (In₂O₃) and polyethylenimine (PEI)‐doped In₂O₃ (In₂O₃:x% PEI, x = 0.5–4.0 wt%) as the channel layer. A two‐dimensional electron gas (2DEG) is thereby achieved by creating a band offset between the In₂O₃ and PEI‐In₂O₃ via work function tuning of the In₂O₃:x% PEI, from 4.00 to 3.62 eV as the PEI content is increased from 0.0 (pristine In₂O₃) to 4.0 wt%, respectively. The resulting devices achieve electron mobilities greater than 10 cm² V^?1 s^?1 on a 300 nm SiO₂ gate dielectric. Importantly, these metrics exceed those of the devices composed of the pristine In₂O₃ materials, which achieve a maximum mobility of ≈4 cm² V^?1 s^?1. Furthermore, a mobility as high as 30 cm² V^?1 s^?1 is achieved on a high‐k ZrO₂ dielectric in the homojunction devices. This is the first demonstration of 2DEG‐based homojunction oxide TFTs via band offset achieved by simple polymer doping of the same MO material.     

High‐Performance Inverted Planar Perovskite Solar Cells Enhanced by Thickness Tuning of New Dopant‐Free Hole Transporting Layer

A new hole transporting material (HTM) named DMZ is synthesized and employed as a dopant‐free HTM in inverted planar perovskite solar cells (PSCs). Systematic studies demonstrate that the thickness of the hole transporting layer can effectively enhance the morphology and crystallinity of the perovskite layer, leading to low series resistance and less defects in the crystal. As a result, the champion power conversion efficiency (PCE) of 18.61% with J_SC = 22.62 mA cm^?2, V_OC = 1.02 V, and FF = 81.05% (an average one is 17.62%) is achieved with a thickness of ≈13 nm of DMZ (2 mg mL^?1) under standard global AM 1.5 illumination, which is ≈1.5 times higher than that of devices based on poly(3,4‐ethylenedioxythiophene)/poly(styrene sulfonic acid) (PEDOT:PSS). More importantly, the devices based on DMZ exhibit a much better stability (90% of maximum PCE retained after more than 556 h in air (relative humidity ≈ 45%–50%) without any encapsulation) than that of devices based on PEDOT:PSS (only 36% of initial PCE retained after 77 h in same conditions). Therefore, the cost‐effective and facile material named DMZ offers an appealing alternative to PEDOT:PSS or polytriarylamine for highly efficient and stable inverted planar PSCs.     

Atomic Cobalt Covalently Engineered Interlayers for Superior Lithium‐Ion Storage

With the unique‐layered structure, MXenes show potential as electrodes in energy‐storage devices including lithium‐ion (Li⁺) capacitors and batteries. However, the low Li⁺‐storage capacity hinders the application of MXenes in place of commercial carbon materials. Here, the vanadium carbide (V₂C) MXene with engineered interlayer spacing for desirable storage capacity is demonstrated. The interlayer distance of pristine V₂C MXene is controllably tuned to 0.735 nm resulting in improved Li‐ion capacity of 686.7 mA h g^?1 at 0.1 A g^?1, the best MXene‐based Li⁺‐storage capacity reported so far. Further, cobalt ions are stably intercalated into the interlayer of V₂C MXene to form a new interlayer‐expanded structure via strong V–O–Co bonding. The intercalated V₂C MXene electrodes not only exhibit superior capacity up to 1117.3 mA h g^?1 at 0.1 A g^?1, but also deliver a significantly ultralong cycling stability over 15 000 cycles. These results clearly suggest that MXene materials with an engineered interlayer distance will be a rational route for realizing them as superstable and high‐performance Li⁺ capacitor electrodes.     

Plant Sunscreen and Co(II)/(III) Porphyrins for UV‐Resistant and Thermally Stable Perovskite Solar Cells: From Natural to Artificial

The poor UV, thermal, and interfacial stability of perovskite solar cells (PSCs) makes it highly challenging for their technological application, and has drawn increasing attention to resolving the above issues. In nature, plants generally sustain long exposure to UV illumination without damage, which is attributed to the presence of the organic materials acting as sunscreens. Inspired by the natural phenomenon, a natural plant sunscreen, sinapoyl malate, an ester derivative of sinapic acid, is employed to modify the surface of electron transport materials (ETMs). The interfacial modification successfully resolved the UV stability and reduced the poor interfacial contact between ETM and perovskite. The best efficiency of fabricated PSCs is up to 19.6%. Furthermore, we employed a mixture of Co(II) and Co(III)‐based porphyrin compounds containing the excellent Co(II)/Co(III) redox couple to substitute the commonly used hole transport material, 2,2′,7,7′‐tetrakis(N,N‐di‐p‐methoxyphenylamine)‐9,9‐spiro‐bifluorene (spiro‐OMeTAD), to resolve the thermal degradation of PSCs noted at and above 80 °C that originates from ion diffusion of I^? and CH₃NH₃⁺ (MA⁺) ions from perovskite into spiro‐OMeTAD. Finally, the stable PSCs with the best efficiency up to 20.5% are successfully fabricated.     

Highly Stable and Efficient FASnI3‐Based Perovskite Solar Cells by Introducing Hydrogen Bonding

Tin‐based perovskites with narrow bandgaps and high charge‐carrier mobilities are promising candidates for the preparation of efficient lead‐free perovskite solar cells (PSCs). However, the crystalline rate of tin‐based perovskites is much faster, leading to abundant trap states and much lower open‐circuit voltage (V_oc). Here, hydrogen bonding is introduced to retard the crystalline rate of the FASnI₃ perovskite. By adding poly(vinyl alcohol) (PVA), the O? H…I^? hydrogen bonding interactions between PVA and FASnI₃ have the effects of introducing nucleation sites, slowing down the crystal growth, directing the crystal orientation, reducing the trap states, and suppressing the migration of the iodide ions. In the presence of the PVA additive, the FASnI₃–PVA PSCs attain higher power conversion efficiency of 8.9% under a reverse scan with significantly improved V_oc from 0.55 to 0.63 V, which is one of the highest V_oc values for FASnI₃‐based PSCs. More importantly, the FASnI₃–PVA PSCs exhibit striking long‐term stability, with no decay in efficiency after 400 h of operation at the maximum power point. This approach, which makes use of the O? H…I^? hydrogen bonding interactions between PVA and FASnI₃, is generally applicable for improving the efficiency and stability of the FASnI₃‐based PSCs.     

Mixed Lead Halide Passivation of Quantum Dots

Infrared‐absorbing colloidal quantum dots (IR CQDs) are materials of interest in tandem solar cells to augment perovskite and cSi photovoltaics (PV). Today's best IR CQD solar cells rely on the use of passivation strategies based on lead iodide; however, these fail to passivate the entire surface of IR CQDs. Lead chloride passivated CQDs show improved passivation, but worse charge transport. Lead bromide passivated CQDs have higher charge mobilities, but worse passivation. Here a mixed lead‐halide (MPbX) ligand exchange is introduced that enables thorough surface passivation without compromising transport. MPbX–PbS CQDs exhibit properties that exceed the best features of single lead‐halide PbS CQDs: they show improved passivation (43 ± 5 meV vs 44 ± 4 meV in Stokes shift) together with higher charge transport (4 × 10^‐2 ± 3 × 10^‐3 cm² V^‐1 s^‐1 vs 3 × 10^‐2 ± 3 × 10^‐3 cm² V^‐1 s^‐1 in mobility). This translates into PV devices having a record IR open‐circuit voltage (IR V_oc) of 0.46 ± 0.01 V while simultaneously having an external quantum efficiency of 81 ± 1%. They provide a 1.7× improvement in the power conversion efficiency of IR photons (>1.1 µm) relative to the single lead‐halide controls reported herein.