Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Use of an Underlayer for Large Area Crystallization of Rubrene Thin Films

Journal Article · · Chemistry of Materials
 [1];  [2];  [3];  [4];  [2];  [4];  [3];  [2]
  1. Princeton Univ., NJ (United States); Princeton University
  2. Princeton Univ., NJ (United States)
  3. Case Western Reserve Univ., Cleveland, OH (United States)
  4. Rutgers Univ., Piscataway, NJ (United States)

In this work, we discovered a very efficient method of crystallization of thermally evaporated rubrene, resulting in ultrathin, large-area, fully connected, and highly crystalline thin films of this organic semiconductor with a grain size of up to 500 μm and charge carrier mobility of up to 3.5 cm2 V–1 s–1. We found that it is critical to use a 5 nm-thick organic underlayer on which a thin film of amorphous rubrene is evaporated and then annealed to dramatically influence the ability of rubrene to crystallize. The underlayer property that controls this influence is the glass transition temperature. By experimenting with different underlayers with glass transition temperatures varying over 120 °C, we identified the molecules leading to the best crystallinity of rubrene films and explained why values both above and below the optimum result in poor crystallinity. We discuss the formation of different crystalline morphologies of rubrene produced by this method and show that field-effect transistors made with films of a single-domain platelet morphology, achieved through the aid of the optimal underlayer, outperform their spherulite counterparts with a nearly four times higher charge carrier mobility. Here, this large-area crystallization technique overcomes the fabrication bottleneck of high-mobility rubrene thin film transistors and other related devices and, given its scalability and patternability, may lead to practical technologies compatible with large-area flexible electronics.

Research Organization:
Princeton Univ., NJ (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Grant/Contract Number:
SC0012458
OSTI ID:
1595412
Alternate ID(s):
OSTI ID: 1534460
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 16 Vol. 29; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (29)

Preparation and Characterization of Blue-Luminescent Tris(8-hydroxyquinoline)-aluminum (Alq3) journal February 2003
High-Performance Organic Photovoltaic Devices Using a New Amorphous Molecular Material with High Hole Drift Mobility, Tris[4-(5-phenylthiophen-2-yl)phenyl]amine journal December 2009
Substrate-Induced and Thin-Film Phases: Polymorphism of Organic Materials on Surfaces journal January 2016
Band-Like Electron Transport in Organic Transistors and Implication of the Molecular Structure for Performance Optimization journal December 2011
Microcrystalline Organic Thin-Film Solar Cells journal August 2013
Estimation of the surface free energy of polymers journal August 1969
Organic molecular beam deposition: Growth studies beyond the first monolayer journal May 2004
Abrupt heating-induced high-quality crystalline rubrene thin films for organic thin-film transistors journal August 2011
Crystal Morphology and Growth in Annealed Rubrene Thin Films journal July 2016
Control of Rubrene Polymorphs via Polymer Binders: Applications in Organic Field-Effect Transistors journal May 2015
Homoepitaxy of Crystalline Rubrene Thin Films journal April 2017
A Quantitative Structure−Property Relationship Study of the Glass Transition Temperature of OLED Materials journal May 2003
Geometric and Electronic Structure of Templated C 60 on Diindenoperylene Thin Films journal January 2013
Optimization of Temperature-Mediated Organic Semiconducting Crystals on Soft Polymer-Treated Gate Dielectrics journal November 2013
Translational and Rotational Motion of Probes in Supercooled 1,3,5-Tris(naphthyl)benzene journal January 1996
Thickness Dependence of the Glass Transition Temperature in Thin Polymer Films journal May 2001
The path to ubiquitous and low-cost organic electronic appliances on plastic journal April 2004
Organic thin-film electronics from vitreous solution-processed rubrene hypereutectics journal July 2005
Observation of long-range exciton diffusion in highly ordered organic semiconductors journal October 2010
Patterning of rubrene thin-film transistors based on electron irradiation of a polystyrene dielectric layer journal January 2015
Effects of film morphology and gate dielectric surface preparation on the electrical characteristics of organic-vapor-phase-deposited pentacene thin-film transistors journal July 2002
Material design of hole transport materials capable of thick-film formation in organic light emitting diodes journal April 2007
Solution-based patterned growth of rubrene nanocrystals for organic field effect transistors journal December 2009
Alternative p-doped hole transport material for low operating voltage and high efficiency organic light-emitting diodes journal September 2014
Nucleation of organic semiconductors on inert substrates journal November 2003
Charge transport and Hall effect in rubrene single-crystal transistors under high pressure journal December 2011
Growth and form of spherulites journal July 2005
Intrinsic Charge Transport on the Surface of Organic Semiconductors journal August 2004
Low-temperature structure of rubrene single crystals grown by vapor transport journal March 2006

Cited By (5)

Hall Effect in Polycrystalline Organic Semiconductors: The Effect of Grain Boundaries journal July 2019
Band-like Charge Photogeneration at a Crystalline Organic Donor/Acceptor Interface journal December 2017
The Impact of Local Morphology on Organic Donor/Acceptor Charge Transfer States journal January 2018
Formation of aligned periodic patterns during the crystallization of organic semiconductor thin films journal June 2019
Oxidation of rubrene, and implications for device stability journal January 2018

Similar Records

Multimodal Characterization of Crystal Structure and Formation in Rubrene Thin Films Reveals Erasure of Orientational Discontinuities
Journal Article · Wed Jan 18 23:00:00 EST 2023 · Advanced Functional Materials · OSTI ID:1963117

Dislocations and Grain Boundaries in Semiconducting Rubrene Single-Crystals
Journal Article · Sat Dec 31 23:00:00 EST 2005 · J. Cryst. Growth · OSTI ID:914389

Homoepitaxy of Crystalline Rubrene Thin Films
Journal Article · Mon Apr 10 00:00:00 EDT 2017 · Nano Letters · OSTI ID:1595415