skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Photovoltaic Diode Effect Induced by Positive Bias Poling of Organic Layer‐Mediated Interface in Perovskite Heterostructure α‐HC(NH 2 ) 2 PbI 3 /TiO 2
It is shown that in the formamidinium (FA) lead iodide/titania heterostructure α‐HC(NH2)2PbI3/TiO2the organic layer‐mediated interface, i.e., FAI/TiO2, can induce photovoltaic diode effect via positive bias poling. The band gap of the heterostructure is reduced to zero upon the positive poling due to combined effects of ion diffusion, rotation of organic moieties, and ferroelectric redistribution. The perovskite part in the organic layer‐mediated interface FAI/TiO2gives rise to a strong polarization of 18.69 μC cm−2, compared to that (0.89 μC cm−2) in the inorganic layer‐mediated interface PbI2/TiO2. The strong polarization of the organic layer‐mediated interface is closely related to the diode effect associated with the reordering of the ferroelectric polarization and charge distribution, as a consequence of the mobility and rotation of organic moieties in FAI/TiO2upon the positive bias poling. The latter effect also provides an explanation on why the FAPbI3‐based devices can largely reduce the scanning hysteresis in theJ–Vcurves (Yang et al.,Science2015,348, 1234) and why the organic layer‐mediated halide perovskite heterostructure is one of the most promising candidates for the fabrication of highly efficient solar cells or optoelectronic devices.  more » « less
Award ID(s):
1538893
PAR ID:
10235557
Author(s) / Creator(s):
 ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials Interfaces
Volume:
3
Issue:
17
ISSN:
2196-7350
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract We report the pulsed‐laser deposition of epitaxial double‐perovskite Bi2FeCrO6(BFCO) films on the (001)‐, (110), and (111)‐oriented single‐crystal SrTiO3substrates. All of the BFCO films with various orientations show theandsuperlattice‐diffraction peaks. The intensity ratios between the‐superlattice and the main 111‐diffraction peak can be tailored by simply adjusting the laser repetition rate and substrate temperature, reaching up to 4.4%. However, both optical absorption spectra and magnetic measurements evidence that the strong superlattice peaks are not correlated with theB‐site Fe3+/Cr3+cation ordering. Instead, the epitaxial (111)‐oriented Bi2FeCrO6films show an enhanced remanent polarization of 92 μC/cm2at 10 K, much larger than the predicted values by density‐functional theory calculations. Positive‐up‐negative‐down (PUND) measurements with a time interval of 10 μs further support these observations. Therefore, our experimental results reveal that the strong superlattice peaks may come fromA‐ orB‐site cation shifts along the pseudo‐cubic [111] direction, which further enhance the ferroelectric polarization of the BFCO thin films. 
    more » « less
  2. null (Ed.)
    The thermal stability and decomposition pathway of formamidinium iodide (FAI, HC(NH 2 ) 2 I) in contact with NiO and TiO 2 are investigated by combined experimental studies and density functional theory (DFT) calculations. Based on the decomposition temperature, we find that the stability decreases as FAI ∼ FAI + TiO 2 > FAI + NiO. Moreover, FAPbI 3 in contact with NiO and TiO 2 shows similar thermal stability behaviour to FAI. The bulk decomposition of FAI occurs via the formation of sym -triazine, and can also produce HCN, and NH 4 I at ∼280 °C, which further decomposes to NH 3 and HI above 300 °C. When FAI comes into contact with NiO, the interfacial reaction triggers decomposition at a much lower temperature (∼200 °C), resulting in the formation of NiI 2 as the solid product while releasing NH 3 and H 2 O into the gas phase; sym -triazine and HCN are observed near the FAI bulk decomposition temperature. In contrast, when FAI comes into contact with TiO 2 , the decomposition temperature is similar to bulk FAI; however, HCN is released at a lower temperature (∼260 °C) compared to sym -triazine. The difference in the degradation behavior of FAI with NiO and TiO 2 is elucidated using DFT calculations. Our results show that the interfacial reaction between the organic component of perovskite material and NiO occurs similarly for MA and FA, which thereby can induce device instability. 
    more » « less
  3. Abstract The Ruddlesden‐Popper 5diridate Sr2IrO4is an antiferromagnetic Mott insulator with the electronic, magnetic, and structural properties highly intertwined. Voltage control of its magnetic state is of intense fundmenatal and technological interest but remains to be demonstrated. Here, the tuning of magnetotransport properties in 5.2 nm Sr2IrO4via interfacial ferroelectric PbZr0.2Ti0.8O3is reported. The conductance of the epitaxial PbZr0.2Ti0.8O3/Sr2IrO4heterostructure exhibits ln(T) behavior that is characteristic of 2D correlated metal, in sharp contrast to the thermally activated behavior followed by 3D variable range hopping observed in single‐layer Sr2IrO4films. Switching PbZr0.2Ti0.8O3polarization induces nonvolatile, reversible resistance modulation in Sr2IrO4. At low temperatures, the in‐plane magnetoresisance in the heterostructure transitions from positive to negative at high magnetic fields, opposite to the field dependence in single‐layer Sr2IrO4. In the polarization down state, the out‐of‐plane anisotropic magnetoresistanceRAMRexhibits sinusoidal angular dependence, with a 90° phase shift below 20 K. For the polarization up state, unusual multi‐level resistance pinning appears inRAMRbelow 30 K, pointing to enhanced magnetocrystalline anisotropy. The work sheds new light on the intriguing interplay of interface lattice coupling, charge doping, magnetoelastic effect, and possible incipient ferromagnetism in Sr2IrO4, facilitating the functional design of its electronic and material properties. 
    more » « less
  4. Air‐stable p‐type SnF2:Cs2SnI6with a bandgap of 1.6 eV has been demonstrated as a promising material for Pb‐free halide perovskite solar cells. Crystalline Cs2SnI6phase is obtained with CsI, SnI2, and SnF2salts in gamma‐butyrolactone solvent, but not with dimethyl sulfoxide andN,N‐dimethylformamide solvents. Cs2SnI6is found to be stable for at least 1000 h at 100 °C when dark annealed in nitrogen atmosphere. In this study, Cs2SnI6has been used in a superstrate n–i–p planar device structure enabled by a spin‐coated absorber thickness of ≈2 μm on a chemical bath deposited Zn(O,S) electron transport layer. The best device power conversion efficiency reported here is 5.18% withVOCof 0.81 V, 9.28 mA cm−2JSC, and 68% fill factor. The dark saturation current and diode ideality factor are estimated as 1.5 × 10−3 mA cm−2and 2.18, respectively. The devices exhibit a highVOCdeficit and low short‐circuit current density due to high bulk and interface recombination. Device efficiency can be expected to increase with improvement in material and interface quality, charge transport, and device engineering. 
    more » « less
  5. Abstract In this work, TiO2thin films deposited by the atomic layer deposition (ALD) method were treated with a special N2O plasma surface treatment and used as the gate dielectric for AlGaN/GaN metal insulator semiconductor high electron mobility transistors (MISHEMTs). The N2O plasma surface treatment effectively reduces defects in the oxide during low-temperature ALD growth. In addition, it allows oxygen atoms to diffuse into the device cap layer to increase the barrier height and thus reduce the gate leakage current. These TiO2films exhibit a dielectric constant of 54.8 and a two-terminal current of 1.96 × 10−10A mm−1in 2μm distance. When applied as the gate dielectric, the AlGaN/GaN MISHEMT with a 2μm-gate-length shows a high on/off ratio of 2.59 × 108and a low subthreshold slope (SS) of 84 mV dec−1among all GaN MISHEMTs using TiO2as the gate dielectric. This work provides a feasible way to significantly improve the TiO2film electrical property for gate dielectrics, and it suggests that the developed TiO2dielectric is a promising high-κgate oxide and a potential passivation layer for GaN-based MISHEMTs, which can be further extended to other transistors. 
    more » « less