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Open Access Publications from the University of California

Scholarly Works (28 results)

  • Thesis
  • Peer Reviewed
UCLA Electronic Theses and Dissertations (2014)

Organic photovoltaic (OPV) devices show great promise in low-cost, flexible, lightweight, and large-area energy-generation applications. Nonetheless, most of the materials designed today always suffer from the inherent disadvantage of not having a broad absorption range, and relatively low mobility, which limit the utilization of the full solar spectrum. Tandem solar cells provide an effective way to harvest a broader spectrum of solar radiation by combining two or more solar cells with different absorption bands. However, for polymer solar cells, the performance of tandem devices lags behind single-layer solar cells mainly due to the lack of suitable low-bandgap polymers (near-IR absorbing polymers). In this dissertation, in order to achieve high performance, we focus on design and synthesis of novel low bandgap polymers specifically for tandem solar cells.

In Chapter 3, I demonstrate highly efficient single junction and tandem polymer solar cells featuring a spectrally matched low-bandgap conjugated polymer (PBDTT-DPP: bandgap, ∼1.44 eV). The polymer has a backbone based on alternating benzodithiophene and diketopyrrolopyrrole units. A single-layer device based on the polymer provides a power conversion efficiency of ∼6%. When the polymer is applied to tandem solar cells, a power conversion efficiency of 8.62% is achieved, which was the highest certified efficiency for a polymer solar cell.

To further improve this material system, in Chapter 4, I show that the reduction of the bandgap and the enhancement of the charge transport properties of the low bandgap polymer PBDTT-DPP can be accomplished simultaneously by substituting the sulfur atoms on the DPP unit with selenium atoms. The newly designed polymer PBDTT-SeDPP (Eg = 1.38 eV) shows excellent photovoltaic performance in single junction devices with PCEs over 7% and photo-response up to 900 nm. Tandem polymer solar cells based on PBDTT-SeDPP are also demonstrated with a 9.5% PCE, which are more than 10% enhancement over those based on PBDTT-DPP.

Finally, in Chapter 5, I demonstrate a new polymer system based on alternating dithienopyran and benzothiadiazole units with a bandgap of 1.38 eV, high mobility, deep highest occupied molecular orbital. As a result, a single-junction device shows high external quantum efficiency of >60% and spectral response that extends to 900 nm, with a power conversion efficiency of 7.9%. The polymer enables a solution processed tandem solar cell with certified 10.6% power conversion efficiency under standard reporting conditions, which is the first certified polymer solar cell efficiency over 10%.

    Cover page: Achieving High Performance Polymer Tandem Solar Cells via Novel Materials Design
    • Article
    • Peer Reviewed
    UC Berkeley Previously Published Works (2017)
    Over the past decade, tremendous progress has been achieved in the development of nanoscale semiconductor materials with a wide range of bandgaps by alloying different individual semiconductors. These materials include traditional II-VI and III-V semiconductors and their alloys, inorganic and hybrid perovskites, and the newly emerging 2D materials. One important common feature of these materials is that their nanoscale dimensions result in a large tolerance to lattice mismatches within a monolithic structure of varying composition or between the substrate and target material, which enables us to achieve almost arbitrary control of the variation of the alloy composition. As a result, the bandgaps of these alloys can be widely tuned without the detrimental defects that are often unavoidable in bulk materials, which have a much more limited tolerance to lattice mismatches. This class of nanomaterials could have a far-reaching impact on a wide range of photonic applications, including tunable lasers, solid-state lighting, artificial photosynthesis and new solar cells.
      Cover page: Bandgap engineering in semiconductor alloy nanomaterials with widely tunable compositions
      • Article
      • Peer Reviewed
      UC Berkeley Previously Published Works (2017)
      A hot phonon bottleneck may be responsible for slow hot carrier cooling in methylammonium lead iodide hybrid perovskite, creating the potential for more efficient hot carrier photovoltaics. In room-temperature 2D electronic spectra near the band edge, we observe amplitude oscillations due to a remarkably long lived 0.9 THz coherent phonon population at room temperature. This phonon (or set of phonons) is assigned to angular distortions of the Pb-I lattice, not coupled to cation rotations. The strong coupling between the electronic transition and the 0.9 THz mode(s), together with relative isolation from other phonon modes, makes it likely to cause a phonon bottleneck. The pump frequency resolution of the 2D spectra also enables independent observation of photoinduced absorptions and bleaches independently and confirms that features due to band gap renormalization are longer-lived than in transient absorption spectra.
        • Article
        • Peer Reviewed
        UC Berkeley Previously Published Works (2015)
        Halide perovskites have attracted much attention over the past 5 years as a promising class of materials for optoelectronic applications. However, compared to hybrid organic-inorganic perovskites, the study of their pure inorganic counterparts, like cesium lead halides (CsPbX3), lags far behind. Here, a catalyst-free, solution-phase synthesis of CsPbX3 nanowires (NWs) is reported. These NWs are single-crystalline, with uniform growth direction, and crystallize in the orthorhombic phase. Both CsPbBr3 and CsPbI3 are photoluminescence active, with composition-dependent temperature and self-trapping behavior. These NWs with a well-defined morphology could serve as an ideal platform for the investigation of fundamental properties and the development of future applications in nanoscale optoelectronic devices based on all-inorganic perovskites.
          Cover page: Solution-Phase Synthesis of Cesium Lead Halide Perovskite Nanowires
          • Article
          • Peer Reviewed
          UCLA Previously Published Works (2019)
          This Article contains an error in Equation 2 in that the denominator is inverted. This has not been fixed in the PDF or HTML versions of the Article but can be seen in the associated Correction.
            Cover page: Author Correction: Solution-processed hybrid perovskite photodetectors with high detectivity
            • Article
            • Peer Reviewed
            UC Berkeley Previously Published Works (2016)
            The radiation-sensitive nature of halide perovskites has hindered structural studies at the atomic scale. We overcome this obstacle by applying low dose-rate in-line holography, which combines aberration-corrected high-resolution transmission electron microscopy with exit-wave reconstruction. This technique successfully yields the genuine atomic structure of ultrathin two-dimensional CsPbBr3 halide perovskites, and a quantitative structure determination was achieved atom column by atom column using the phase information of the reconstructed exit-wave function without causing electron beam-induced sample alterations. An extraordinarily high image quality enables an unambiguous structural analysis of coexisting high-temperature and low-temperature phases of CsPbBr3 in single particles. On a broader level, our approach offers unprecedented opportunities to better understand halide perovskites at the atomic level as well as other radiation-sensitive materials.
              Cover page: Atomic Resolution Imaging of Halide Perovskites
              • Article
              • Peer Reviewed
              UC Berkeley Previously Published Works (2017)
              Cesium lead iodide (CsPbI3), in its black perovskite phase, has a suitable bandgap and high quantum efficiency for photovoltaic applications. However, CsPbI3 tends to crystalize into a yellow non-perovskite phase, which has poor optoelectronic properties, at room temperature. Therefore, controlling the phase transition in CsPbI3 is critical for practical application of this material. Here we report a systematic study of the phase transition of one-dimensional CsPbI3 nanowires and their corresponding structural, optical, and electrical properties. We show the formation of perovskite black phase CsPbI3 nanowires from the non-perovskite yellow phase through rapid thermal quenching. Post-transformed black phase CsPbI3 nanowires exhibit increased photoluminescence emission intensity with a shrinking of the bandgap from 2.78 to 1.76 eV. The perovskite nanowires were photoconductive and showed a fast photoresponse and excellent stability at room temperature. These promising optical and electrical properties make the perovskite CsPbI3 nanowires attractive for a variety of nanoscale optoelectronic devices. [Figure not available: see fulltext.]
                Cover page: Structural, optical, and electrical properties of phase-controlled cesium lead iodide nanowires
                • Article
                • Peer Reviewed
                UC Berkeley Previously Published Works (2015)
                Colloidal metal nanowire based transparent conductors are excellent candidates to replace indium-tin-oxide (ITO) owing to their outstanding balance between transparency and conductivity, flexibility, and solution-processability. Copper stands out as a promising material candidate due to its high intrinsic conductivity and earth abundance. Here, we report a new synthetic approach, using tris(trimethylsilyl)silane as a mild reducing reagent, for synthesizing high-quality, ultrathin, and monodispersed copper nanowires, with an average diameter of 17.5 nm and a mean length of 17 μm. A study of the growth mechanism using high-resolution transmission electron microscopy reveals that the copper nanowires adopt a five-fold twinned structure and evolve from decahedral nanoseeds. Fabricated transparent conducting films exhibit excellent transparency and conductivity. An additional advantage of our nanowire transparent conductors is highlighted through reduced optical haze factors (forward light scattering) due to the small nanowire diameter.
                  Cover page: Synthesis of Ultrathin Copper Nanowires Using Tris(trimethylsilyl)silane for High-Performance and Low-Haze Transparent Conductors
                  • Article
                  • Peer Reviewed
                  UC Berkeley Previously Published Works (2018)
                  Alloying different semiconductors is a powerful approach to tuning the optical and electronic properties of semiconductor materials. In halide perovskites (ABX3), alloys with different anions have been widely studied, and great band gap tunability in the visible range has been achieved. However, perovskite alloys with different cations at the "B" site are less understood due to the synthetic challenges. Herein, we first have developed the synthesis of single-crystalline CsPb xSn1- xI3 nanowires (NWs). The electronic band gaps of CsPb xSn1- xI3 NWs can be tuned from 1.3 to 1.78 eV by varying the Pb/Sn ratio, which leads to the tunable photoluminescence (PL) in the near-infrared range. More importantly, we found that the electrical conductivity increases as more Sn2+ is alloyed with Pb2+, possibly due to the increase of charge carrier concentration when more Sn2+ is introduced. The wide tunability of the optical and electronic properties makes CsPb xSn1- xI3 alloy NWs promising candidates for future optoelectronic device applications.
                    Cover page: Electrical and Optical Tunability in All-Inorganic Halide Perovskite Alloy Nanowires
                    • Article
                    • Peer Reviewed
                    UCLA Previously Published Works (2013)
                    A two-dimensional conjugated small molecule (SMPV1) was designed and synthesized for high performance solution-processed organic solar cells. This study explores the photovoltaic properties of this molecule as a donor, with a fullerene derivative as an acceptor, using solution processing in single junction and double junction tandem solar cells. The single junction solar cells based on SMPV1 exhibited a certified power conversion efficiency of 8.02% under AM 1.5 G irradiation (100 mW cm(-2)). A homo-tandem solar cell based on SMPV1 was constructed with a novel interlayer (or tunnel junction) consisting of bilayer conjugated polyelectrolyte, demonstrating an unprecedented PCE of 10.1%. These results strongly suggest solution-processed small molecular materials are excellent candidates for organic solar cells.
                      Cover page: Solution-processed small-molecule solar cells: breaking the 10% power conversion efficiency
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