Tejas A. Shastry

Polychiral semiconducting carbon nanotube-fullerene solar cells

Single-walled carbon nanotubes (SWCNTs) have highly desirable attributes for solution-processable thin-film photovoltaics (TFPVs), such as broadband absorption, high carrier mobility, and environmental stability. However, previous TFPVs incorporating photoactive SWCNTs have utilized architectures that have limited current, voltage, and ultimately power conversion efficiency (PCE). Here, we report a solar cell geometry that maximizes photocurrent using polychiral SWCNTs while retaining high photovoltage, leading to record-high efficiency SWCNT-fullerene solar cells with average NREL certified and champion PCEs of 2.5% and 3.1%, respectively. Moreover, these cells show significant absorption in the near-infrared portion of the solar spectrum that is currently inaccessible by many leading TFPV technologies.

Broad‐Spectral‐Response Nanocarbon Bulk‐Heterojunction Excitonic Photodetectors

High-performance broad-spectrum nanocarbon bulk-heterojunction photovoltaic photodetectors are reported. These reported photodetectors consist of a semiconducting single-walled carbon nanotube (s-SWCNT) and a PC71 BM blended active layer. Magnetic-field effects and the chirality of the s-SWCNTs play an important role in controlling the photoresponse time and photocurrent improvement.

Large‐Area, Electronically Monodisperse, Aligned Single‐Walled Carbon Nanotube Thin Films Fabricated by Evaporation‐Driven Self‐Assembly

By varying the evaporation conditions and the nanotube and surfactant concentrations, large-area, aligned single-walled carbon nanotube (SWCNT) thin films are fabricated from electronically monodisperse SWCNT solutions by evaporation-driven self-assembly with precise control over the thin film growth geometry. Tunability is possible from 0.5 μm stripes to continuous thin films. The resulting SWCNT thin films possess highly anisotropic electrical and optical properties that are well suited for transparent conductor applications.

Probing carbon nanotube-surfactant interactions with two-dimensional DOSY NMR

Two-dimensional diffusion ordered spectroscopy (2D DOSY) NMR was used to probe the micellar structure of sodium dodecyl sulfate (SDS) and sodium cholate (SC) in aqueous solutions with and without semiconducting and metallic single-walled carbon nanotubes (SWCNTs). The solutions contain SDS and SC at weight ratios of 1:4 and 3:2, the ratios commonly used to isolate semiconducting and metallic SWCNTs through density gradient ultracentrifugation (DGU). These results show that the coverage of surfactant on the semiconducting and metallic SWCNTs is nearly identical in the 1:4 surfactant mixture, and a lower degree of bundling is responsible for the greater buoyancy of semiconducting SWCNTs. In the 3:2 surfactant mixture, the metallic SWCNTs are only encapsulated in SC while the semiconducting SWCNTs remain encapsulated in a poorly packed two-surfactant micelle, leading to a large buoyant density difference between the electronic species. This work provides insight into future directions to increase the purity of semiconducting and metallic SWCNTs sorted through DGU and demonstrates the utility of 2D DOSY NMR in probing SWCNT-surfactant complexes.

Narrow diameter distributions of metallic arc discharge single-walled carbon nanotubes via dual-iteration density gradient ultracentrifugation

The outstanding electrical and mechanical properties of single-walled carbon nanotube (SWCNT) thin fi lms [ 1 ] have brought them to the forefront of materials research for a variety of applications including transparent conductors. [ 2–4 ] While as-produced SWCNT samples inherently contain a variety of tube diameters and chiral angles, leading to a mixture of metallic and semiconducting tubes that presents challenges for practical electronic applications, density gradient ultra-centrifugation (DGU) has enabled the isolation of large quantities of electronically monodisperse material. [ 5 ] Transparent conducting fi lms fabricated using DGU-sorted SWCNTs have been well-characterized [ 6–8 ] and the advantages of using monodisperse metallic SWCNTs have been demonstrated in devices such as organic photovoltaics. [ 9 ] However, these metallic SWCNT samples are comprised of several species with varying diameters and thus exhibit broad optical transitions, which both hinder optoelectronic applications where sharp spectral features are required and impede empirical studies aimed at elucidating the dependence of SWCNT properties on nanotube diameter. Efforts to further refi ne electronically sorted SWCNTs by diameter have typically relied on using starting material from different fabrication techniques such as high pressure carbon monoxide conversion (HiPCO), [ 10 ] laser ablation, [ 11 ] and electric arc discharge [ 12 ] that, when sorted via DGU, provide electronically monodisperse SWCNTs centered about a different tube diameter according to the synthesis method [ 5 , 6 , 13 , 14 ] and/ or batch. [ 15 ] More recent separation techniques that are able to target single ( n , m ) semiconducting species have focused on small-diameter CVD-grown SWCNTs and have not yet distinguished between metallic species of different diameters. [ 16–18 ]

Mutual Photoluminescence Quenching and Photovoltaic Effect in Large-Area Single-Layer MoS2-Polymer Heterojunctions

Two-dimensional transition metal dichalcogenides (TMDCs) have recently attracted attention due to their superlative optical and electronic properties. In particular, their extraordinary optical absorption and semiconducting band gap have enabled demonstrations of photovoltaic response from heterostructures composed of TMDCs and other organic or inorganic materials. However, these early studies were limited to devices at the micrometer scale and/or failed to exploit the unique optical absorption properties of single-layer TMDCs. Here we present an experimental realization of a large-area type-II photovoltaic heterojunction using single-layer molybdenum disulfide (MoS2) as the primary absorber, by coupling it to the organic π-donor polymer PTB7. This TMDC-polymer heterojunction exhibits photoluminescence intensity that is tunable as a function of the thickness of the polymer layer, ultimately enabling complete quenching of the TMDC photoluminescence. The strong optical absorption in the TMDC-polymer heterojunction produces an internal quantum efficiency exceeding 40% for an overall cell thickness of less than 20 nm, resulting in exceptional current density per absorbing thickness in comparison to other organic and inorganic solar cells. Furthermore, this work provides insight into the recombination processes in type-II TMDC-polymer heterojunctions and thus provides quantitative guidance to ongoing efforts to realize efficient TMDC-based solar cells.

Multiferroicity of Carbon‐Based Charge‐Transfer Magnets

A new type of carbon charge-transfer magnet, consisting of a fullerene acceptor and single-walled carbon nanotube donor, is demonstrated, which exhibits room temperature ferromagnetism and magnetoelectric (ME) coupling. In addition, external stimuli (electric/magnetic/elastic field) and the concentration of a nanocarbon complex enable the tunabilities of the magnetization and ME coupling due to the control of the charge transfer.

Improved uniformity in high-performance organic photovoltaics enabled by (3-aminopropyl)triethoxysilane cathode functionalization

Organic photovoltaics have the potential to serve as lightweight, low-cost, mechanically flexible solar cells. However, losses in efficiency as laboratory cells are scaled up to the module level have to date impeded large scale deployment. Here, we report that a 3-aminopropyltriethoxysilane (APTES) cathode interfacial treatment significantly enhances performance reproducibility in inverted high-efficiency PTB7:PC71BM organic photovoltaic cells, as demonstrated by the fabrication of 100 APTES-treated devices versus 100 untreated controls. The APTES-treated devices achieve a power conversion efficiency of 8.08 ± 0.12% with histogram skewness of -0.291, whereas the untreated controls achieve 7.80 ± 0.26% with histogram skewness of -1.86. By substantially suppressing the interfacial origins of underperforming cells, the APTES treatment offers a pathway for fabricating large-area modules with high spatial performance uniformity.

Charge-Transfer Induced Magnetic Field Effects of Nano-Carbon Heterojunctions

Room temperature magnetic field effects have not been definitively observed in either single-walled carbon nanotubes (SWCNTs) or C60 under a small magnetic field due to their weak hyperfine interaction and slight difference of g-factor between positive and negative polarons. Here, we demonstrate charge-transfer induced magnetic field effects in nano-carbon C60-SWCNT bulk heterojunctions at room temperature, where the mechanism of magnetic field effects is verified using excited state transition modeling. By controlling SWCNT concentrations and interfacial interactions, nano-carbon heterojunctions exhibit tunability of charge-transfer density and room temperature magnetoconductance of 2.8% under 100 mT external magnetic field. External stimuli, such as electric field and photoexcitation, also play an important role in controlling the magnetic field effects of nano-carbon heterojunctions, which suggests that these findings could enable the control of optoelectronic properties of nano-carbon heterojunctions.

Understanding charge transfer in carbon nanotube-fullerene bulk heterojunctions.

Semiconducting single-walled carbon nanotube/fullerene bulk heterojunctions exhibit unique optoelectronic properties highly suitable for flexible, efficient, and robust photovoltaics and photodetectors. We investigate charge-transfer dynamics in inverted devices featuring a polyethylenimine-coated ZnO nanowire array infiltrated with these blends and find that trap-assisted recombination dominates transport within the blend and at the active layer/nanowire interface. We find that electrode modifiers suppress this recombination, leading to high performance.