Xiaokai Li

Record High Efficiency Single-Walled Carbon Nanotube/Silicon p–n Junction Solar Cells

Carrier transport characteristics in high-efficiency single-walled carbon nanotubes (SWNTs)/silicon (Si) hybrid solar cells are presented. The solar cells were fabricated by depositing intrinsic p-type SWNT thin-films on n-type Si wafers without involving any high-temperature process for p-n junction formation. The optimized cells showed a device ideality factor close to unity and a record-high power-conversion-efficiency of >11%. By investigating the dark forward current density characteristics with varying temperature, we have identified that the temperature-dependent current rectification originates from the thermally activated band-to-band transition of carriers in Si, and the role of the SWNT thin films is to establish a built-in potential for carrier separation/collection. We have also established that the dominant carrier transport mechanism is diffusion, with minimal interface recombination. This is further supported by the observation of a long minority carrier lifetime of ~34 μs, determined by the transient recovery method. This study suggests that these hybrid solar cells operate in the same manner as single crystalline p-n homojunction Si solar cells.

Scalable Fabrication of Multifunctional Freestanding Carbon Nanotube/Polymer Composite Thin Films for Energy Conversion

Translating the unique properties of individual single-walled carbon nanotubes (SWNTs) to the macroscale while simultaneously incorporating additional functionalities into composites has been stymied by inadequate assembly methods. Here we describe a technique for developing multifunctional SWNT/polymer composite thin films that provides a fundamental engineering basis to bridge the gap between their nano- and macroscale properties. Selected polymers are infiltrated into a Mayer rod coated conductive SWNT network to fabricate solar cell transparent conductive electrodes (TCEs), fuel cell membrane electrode assemblies (MEAs), and lithium ion battery electrodes. Our TCEs have an outstanding optoelectronic figure of merit σ(dc)/σ(ac) of 19.4 and roughness of 3.8 nm yet are also mechanically robust enough to withstand delamination, a step toward scratch resistance necessary for flexible electronics. Our MEAs show platinum utilization as high as 1550 mW/mg(Pt), demonstrating our techniques ability to integrate ionic conductivity of the polymer with electrical conductivity of the SWNTs at the Pt surface. Our battery anodes, which show reversible capacity of ∼850 mAh/g after 15 cycles, demonstrate the integration of electrode and separator to simplify device architecture and decrease overall weight. Each of these applications demonstrates our techniques ability to maintain the conductivity of SWNT networks and their dispersion within a polymer matrix while concurrently optimizing key complementary properties of the composite. Here, we lay the foundation for the assembly of nanotubes and nanostructured components (rods, wires, particles, etc.) into macroscopic multifunctional materials using a low-cost and scalable solution-based processing technique.

Improved efficiency of smooth and aligned single walled carbon nanotube/silicon hybrid solar cells

Smooth and aligned single walled carbon nanotube (SWNT) thin films with improved optoelectronic performance are fabricated using a superacid slide casting method. Deposition of as made SWNT thin film on silicon (Si) together with post treatments result in SWNT/Si hybrid solar cells with unprecedented high fill factor of 73.8%, low ideality factor of 1.08 as well as overall dry cell power conversion efficiency of 11.5%.

Improving the assembly speed, quality, and tunability of thin conductive multilayers.

While inhomogeneous thin conductive films have been sought after for their flexibility, transparency, and strength, poor control in the processing of these materials has restricted their application. The versatile layer-by-layer assembly technique allows greater control over film deposition, but even this has been hampered by the traditional dip-coating method. Here, we employ a fully automated spin-spray layer-by-layer system (SSLbL) to rapidly produce high-quality, tunable multilayer films. With bilayer deposition cycle times as low as 13 s (~50% of previously reported) and thorough characterization of film conductance in the near percolation region, we show that SSLbL permits nanolevel control over film growth and efficient formation of a conducting network not available with other methods of multilayer deposition. The multitude of variables from spray time, to spin rate, to active drying available with SSLbL makes films generated by this technique inherently more tunable and expands the opportunity for optimization and application of composite multilayers. A comparison of several polymer-CNT systems deposited by both spin-spray and dip-coating exemplifies the potential of SSLbL assembly to allow for rapid screening of multilayer films. Ultrathin polymer-CNT multilayers assembled by SSLbL were also evaluated as lithium-ion battery electrodes, emphasizing the practical application of this technique.

Controlled doping of carbon nanotubes with metallocenes for application in hybrid carbon nanotube/Si solar cells.

There is considerable interest in the controlled p-type and n-type doping of carbon nanotubes (CNT) for use in a range of important electronics applications, including the development of hybrid CNT/silicon (Si) photovoltaic devices. Here, we demonstrate that easy to handle metallocenes and related complexes can be used to both p-type and n-type dope single-walled carbon nanotube (SWNT) thin films, using a simple spin coating process. We report n-SWNT/p-Si photovoltaic devices that are >450 times more efficient than the best solar cells of this type currently reported and show that the performance of both our n-SWNT/p-Si and p-SWNT/n-Si devices is related to the doping level of the SWNT. Furthermore, we establish that the electronic structure of the metallocene or related molecule can be correlated to the doping level of the SWNT, which may provide the foundation for controlled doping of SWNT thin films in the future.

Role of HF in oxygen removal from carbon nanotubes: implications for high performance carbon electronics.

Oxygen removal from SWNTs is crucial for many carbon electronic devices. This work shows that HF treatment followed by current stimulation is a very effective method for oxygen removal. Using a procedure involving HF treatment, current stimulation and spin-casting AgNWs onto a SWNT thin film, record high efficiency SWNT/p-Si solar cells have been developed.

Improving the Performance of P3HT/PCBM Solar Cells with Squaraine Dye

Expanding the spectral absorption breadth and efficiently harvesting excitons are crucial towards creating highly efficient polymer solar cells. Here we describe a strategy to realize broad-band light harvesting in poly(3-hexylthiophene) (P3HT)-based solar cells. We introduce the use of squaraine dye molecules that play a dual role towards improving P3HT-based solar cells. The first benefit is an increase in the spectral absorption in the near infrared region. The second advantage is the collection of excitons close to the interfacial heterojunctions via Förster resonance energy transfer (FRET). Unlike traditional multi-blend systems, where each donor works independently in separate spectral responses, FRET-based systems enable the effective use of multiple donors with significant improvements in light absorption and conversion. Ultrafast transient absorption experiments show that the excitation energy from P3HT can be transferred rapidly (within a few picoseconds) and efficiently (up to 96%) to the squaraine via FRET. As a result, the overall power conversion efficiency is improved. This architecture opens up a new paradigm towards transformative improvements of polymer solar cells.

Charge Transfer from Carbon Nanotubes to Silicon in Flexible Carbon Nanotube/Silicon Solar Cells

Mechanical fragility and insufficient light absorption are two major challenges for thin flexible crystalline Si-based solar cells. Flexible hybrid single-walled carbon nanotube (SWNT)/Si solar cells are demonstrated by applying scalable room-temperature processes for the fabrication of solar-cell components (e.g., preparation of SWNT thin films and SWNT/Si p-n junctions). The flexible SWNT/Si solar cells present an intrinsic efficiency ≈7.5% without any additional light-trapping structures. By using these solar cells as model systems, the charge transport mechanisms at the SWNT/Si interface are investigated using femtosecond transient absorption. Although primary photon absorption occurs in Si, transient absorption measurements show that SWNTs also generate and inject excited charge carriers to Si. Such effects can be tuned by controlling the thickness of the SWNTs. Findings from this study could open a new pathway for designing and improving the efficiency of photocarrier generation and absorption for high-performance ultrathin hybrid SWNT/Si solar cells.