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Title: Trap-Filling Magnetoconductance as an Initialization and Readout Mechanism of Triplet Exciton Spins

Journal Article · · Journal of Physical Chemistry Letters
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]
  1. Colorado School of Mines, Golden, CO (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  2. National Renewable Energy Laboratory (NREL), Golden, CO (United States)
  3. University of Colorado, Boulder, CO (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Photoexcited triplet states are promising candidates for hybrid qubit systems, as they can be used as a controlling gate for nuclear spins. But microwave readout schemes do not generally offer the sensitivity needed to approach the single-molecule limit or the scope to integrate such systems into devices. In this report we demonstrate the possibility of electrical readout of triplet spins at room temperature through a specific mechanism of magnetoconductance (MC) in polycrystalline pentacene. We show that hole-only pentacene devices exhibit a positive photoinduced MC response that is consistent with a trap-filling mechanism. Spin and magnetic-field-dependent quenching of photogenerated triplets by holes quantitatively explains the MC response we observe. These results are distinct in both sign and proposed mechanism compared to previous reports on polyacene materials and provide clear design rules for future spintronic devices based on this spin-sensing mechanism.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Laboratory Directed Research and Development (LDRD) Program; National Science Foundation (NSF)
Grant/Contract Number:
AC36-08GO28308; DGE-2125899
OSTI ID:
1900009
Report Number(s):
NREL/JA-5900-83379; MainId:84152; UUID:59954025-fcbd-4d53-b070-8393dd66d125; MainAdminID:68065
Journal Information:
Journal of Physical Chemistry Letters, Vol. 13, Issue 42; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (74)

Probing the C 60 triplet state coupling to nuclear spins inside and out
  • Filidou, Vasileia; Mamone, Salvatore; Simmons, Stephanie
  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 371, Issue 1998 https://doi.org/10.1098/rsta.2012.0475
journal September 2013
Comparative analysis of magnetic resonance in the polaron pair recombination and the triplet exciton-polaron quenching models journal January 2018
Sub-50 picosecond to microsecond carrier transport dynamics in pentacene thin films journal October 2018
Triplet-exciton quenching in organic phosphorescent light-emitting diodes with Ir-based emitters journal March 2007
Theoretical study of dynamic electron-spin-polarization via the doublet-quartet quantum-mixed state (II). Population transfer and magnetic field dependence of the spin polarization journal January 2012
Enhancement of organic magnetoresistance by electrical conditioning journal May 2008
Potential for spin-based information processing in a thin-film molecular semiconductor journal October 2013
Investigating the influence of traps on organic magnetoresistance by molecular doping journal February 2014
A review on organic spintronic materials and devices: II. Magnetoresistance in organic spin valves and spin organic light emitting diodes journal September 2016
Direct evidence for the electron–hole pair mechanism by studying the organic magneto-electroluminescence based on charge-transfer states journal October 2012
Effect of excited states and applied magnetic fields on the measured hole mobility in an organic semiconductor journal August 2010
Magneto-conductance characteristics of trapped triplet–polaron and triplet–trapped polaron interactions in anthracene-based organic light emitting diodes journal January 2016
Correlated magnetic field effects on carriers and excitons in single-carrier exciplex-based organic photodiodes journal January 2019
Morphology independent triplet formation in pentalene films: Singlet fission as the triplet formation mechanism journal September 2019
Quenching effects in organic electrophosphorescence journal December 2002
Magneto-Conductance in Tri-(8-Hydroxyquinoline) Aluminum-Based Organic Light Emitting Diodes journal August 2013
Magnetic-Field Dependence of the Electroluminescence of Organic Light-Emitting Diodes: A Competition between Exciton Formation and Spin Mixing journal May 2011
Picosecond timescale tracking of pentacene triplet excitons with chemical sensitivity journal June 2019
A two-site bipolaron model for organic magnetoresistance journal April 2008
Magnetoresistance and efficiency measurements of Al q 3 -based OLEDs journal March 2007
Charge Transport Study of 2,2',7,7'-Tetrakis(N,N-di-4-methoxyphenyl amino)-9,9'-spirobifluorene Using Impedance Spectroscopy journal June 2011
Experimental investigation on the origin of magneto-conductance and magneto-electroluminescence in organic light emitting devices journal June 2013
Spin routes in organic semiconductors journal August 2009
Charged Frenkel excitons in organic crystals journal October 2001
An EPR study of the triplet state of pentacene by electron spin-echo techniques and laser flash excitation journal March 1980
Hole-exciton interaction induced high field decay of magneto-electroluminescence in Alq3-based organic light-emitting diodes at room temperature journal January 2016
Polaron-pair generation in poly(phenylene vinylenes) journal October 1992
Role of triplet-doublet quenching in organic magnetoconductance journal November 2018
Pentacene Dimers as a Critical Tool for the Investigation of Intramolecular Singlet Fission journal March 2018
Electron-hole pair mechanism for the magnetic field effect in organic light emitting diodes based on poly(paraphenylene vinylene) journal December 2009
Correlation between bias-dependent ESR signals and magnetic field effects in organic light emitting diodes journal March 2019
Shallow trap states in pentacene thin films from molecular sliding journal April 2005
Hole-limiting conductive vinyl copolymers for AlQ3-based OLED applications journal September 2009
Large magnetoresistance in nonmagnetic π -conjugated semiconductor thin film devices journal November 2005
Tuning the Performance of Organic Spintronic Devices Using X-Ray Generated Traps journal August 2012
Magnetic Field Effect on Triplet Exciton Quenching in Organic Crystals journal August 1968
Electrical Detection of Singlet Fission in Single Crystal Tetracene Transistors journal January 2019
Photoinduced negative magnetoresistance in 6,13-bis(triisopropylsilylethynyl)-pentacene field-effect transistors journal March 2012
Microscopic modeling of magnetic-field effects on charge transport in organic semiconductors journal August 2011
The rise of organic magnetoresistance: materials and challenges journal January 2017
Negative magnetoresistance of organic field effect transistors journal August 2007
Revealing the Nature of Singlet Fission under the Veil of Internal Conversion journal January 2020
Inversion of Magnetoresistance in Organic Semiconductors journal February 2008
Traps and trions as origin of magnetoresistance in organic semiconductors journal July 2013
Charge transport properties in pentacene films: Evaluation of carrier mobility by different techniques journal March 2012
Recombination of polaron and exciton in conjugated polymers journal December 2009
Bipolaron Mechanism for Organic Magnetoresistance journal November 2007
Magnetic Field Effects in π -Conjugated Polymer-Fullerene Blends: Evidence for Multiple Components journal December 2008
Magnetic hyperfine modulation of charge photogeneration in solid films of Alq3 journal September 2003
Identifying the magnetoconductance responses by the induced charge transfer complex states in pentacene-based diodes journal July 2012
Magnetic-field effects in illuminated tetracene field-effect transistors journal February 2012
Oxygen-related traps in pentacene thin films: Energetic position and implications for transistor performance journal July 2008
Separating Positive and Negative Magnetoresistance in Organic Semiconductor Devices journal December 2007
Coherent Spin Manipulation in Molecular Semiconductors: Getting a Handle on Organic Spintronics journal July 2010
Localized trions in conjugated polymers journal December 2007
ENDOR of organic triplet- and quartet-state molecules in liquid solutions and in rigid media journal November 1978
Anomalous room temperature magnetoresistance in organic semiconductors journal May 2006
Molecular spintronics journal January 2011
Zero-field magnetic resonance of the photo-excited triplet state of pentacene at room temperature journal December 2000
Control Over Ligand Exchange Reactivity in Hole Transport Layer Enables High-Efficiency Colloidal Quantum Dot Solar Cells journal January 2021
Triplet-Polaron Quenching in Conjugated Polymers journal October 2007
Unraveling the temperature and voltage dependence of magnetic field effects in organic semiconductors journal November 2013
Coherent Storage of Photoexcited Triplet States UsingSi29Nuclear Spins in Silicon journal February 2012
Organic Spin Valves: A Review journal March 2016
Exploring the validity and limitations of the Mott–Gurney law for charge-carrier mobility determination of semiconducting thin-films journal February 2018
Pulsed electron nuclear double resonance studies of the photoexcited triplet state of pentacene in p-terphenyl crystals at room temperature journal September 2007
Photoinduced magnetoresistance in organic field-effect transistors journal February 2011
Experimental observation of oxygen-related defect state in pentacene thin films journal February 2007
Organic Single-Crystal Spintronics: Magnetoresistance Devices with High Magnetic-Field Sensitivity journal July 2019
Colloidal Quantum Dot Solar Cell Band Alignment using Two-Step Ionic Doping journal October 2020
The magnetic filed effect of the singlet fission reaction in polycrystalline tetracene-based diodes conference August 2021
Ultrafast entangling gates between nuclear spins using photoexcited triplet states journal July 2012
Magnetoconductance responses of triplet polaron pair charge reaction in hyperfine coupling regime journal December 2013
Stimulated Electron Spin Polarization in Strongly Coupled Triplet–Doublet Spin Pairs journal January 2011