skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors

Abstract

3D printing of materials with active functional groups can provide custom-designed structures that promote chemical conversions. Herein, catalytically active architectures were produced by photopolymerizing bifunctional molecules using a commercial stereolithographic 3D printer. Functionalities in the monomers included a polymerizable vinyl group to assemble the 3D structures and a secondary group to provide them with active sites. The 3D-printed architectures containing accessible carboxylic acid, amine, and copper carboxylate functionalities were catalytically active for the Mannich, aldol, and Huisgen cycloaddition reactions, respectively. The functional groups in the 3D-printed structures were also amenable to post-printing chemical modification. As proof of principle, chemically active cuvette adaptors were 3D printed and used to measure in situ the kinetics of a heterogeneously catalyzed Mannich reaction in a conventional solution spectrophotometer. In addition, 3D-printed millifluidic devices with catalytically active copper carboxylate complexes were used to promote azide-alkyne cycloaddition under flow conditions. The importance of controlling the 3D architecture of the millifluidic devices was evidenced by enhancing reaction conversion upon increasing the complexity of the 3D prints.

Authors:
 [1];  [2]
  1. Ames Lab., Ames, IA (United States)
  2. Ames Lab., Ames, IA (United States); Delft Univ. of Technology (Netherlands)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1368055
Alternate Identifier(s):
OSTI ID: 1363711
Report Number(s):
IS-J 9350
Journal ID: ISSN 2469-9950; PRBMDO; TRN: US1702749
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 21; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 3D printing; additive manufacturing; catalysis; polymeric materials; millifluidics

Citation Formats

Mkhitaryan, V. V., and Dobrovitski, V. V. Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.95.214204.
Mkhitaryan, V. V., & Dobrovitski, V. V. Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors. United States. doi:10.1103/PhysRevB.95.214204.
Mkhitaryan, V. V., and Dobrovitski, V. V. Mon . "Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors". United States. doi:10.1103/PhysRevB.95.214204. https://www.osti.gov/servlets/purl/1368055.
@article{osti_1368055,
title = {Quantum dynamics of nuclear spins and spin relaxation in organic semiconductors},
author = {Mkhitaryan, V. V. and Dobrovitski, V. V.},
abstractNote = {3D printing of materials with active functional groups can provide custom-designed structures that promote chemical conversions. Herein, catalytically active architectures were produced by photopolymerizing bifunctional molecules using a commercial stereolithographic 3D printer. Functionalities in the monomers included a polymerizable vinyl group to assemble the 3D structures and a secondary group to provide them with active sites. The 3D-printed architectures containing accessible carboxylic acid, amine, and copper carboxylate functionalities were catalytically active for the Mannich, aldol, and Huisgen cycloaddition reactions, respectively. The functional groups in the 3D-printed structures were also amenable to post-printing chemical modification. As proof of principle, chemically active cuvette adaptors were 3D printed and used to measure in situ the kinetics of a heterogeneously catalyzed Mannich reaction in a conventional solution spectrophotometer. In addition, 3D-printed millifluidic devices with catalytically active copper carboxylate complexes were used to promote azide-alkyne cycloaddition under flow conditions. The importance of controlling the 3D architecture of the millifluidic devices was evidenced by enhancing reaction conversion upon increasing the complexity of the 3D prints.},
doi = {10.1103/PhysRevB.95.214204},
journal = {Physical Review B},
number = 21,
volume = 95,
place = {United States},
year = {2017},
month = {6}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Erratum: Spin routes in organic semiconductors
journal, September 2009

  • Dediu, V. Alek; Hueso, Luis E.; Bergenti, Ilaria
  • Nature Materials, Vol. 8, Issue 10
  • DOI: 10.1038/nmat2544

Tunnel magnetoresistance in organic spin valves in the regime of multistep tunneling
journal, November 2013


Theory for Spin Diffusion in Disordered Organic Semiconductors
journal, April 2009


Modelling decoherence in quantum spin systems
journal, February 2007

  • Zhang, Wenxian; Konstantinidis, N.; Al-Hassanieh, K. A.
  • Journal of Physics: Condensed Matter, Vol. 19, Issue 8
  • DOI: 10.1088/0953-8984/19/8/083202

Tunneling anisotropic magnetoresistance in organic spin valves
journal, September 2011


Monte Carlo Simulation of Quantum Spin Systems. I
journal, November 1977

  • Suzuki, M.; Miyashita, S.; Kuroda, A.
  • Progress of Theoretical Physics, Vol. 58, Issue 5
  • DOI: 10.1143/PTP.58.1377

Spin-Flip Induced Magnetoresistance in Positionally Disordered Organic Solids
journal, May 2012


Room temperature spin polarized injection in organic semiconductor
journal, April 2002


Magnetoresistance in Hybrid Organic Spin Valves at the Onset of Multiple-Step Tunneling
journal, October 2009


Spintronics goes plastic
journal, November 2007


Numerical Modeling of the Central Spin Problem Using the Spin-Coherent-State P Representation
journal, July 2006


Spin-Orbit Coupling, Spin Relaxation, and Spin Diffusion in Organic Solids
journal, March 2011


Hyperfine interaction and magnetoresistance in organic semiconductors
journal, July 2006


Isotope effect in spin response of π-conjugated polymer films and devices
journal, February 2010

  • Nguyen, Tho D.; Hukic-Markosian, Golda; Wang, Fujian
  • Nature Materials, Vol. 9, Issue 4
  • DOI: 10.1038/nmat2633

Giant magnetoresistance in organic spin-valves
journal, February 2004


Hyperfine-Field-Mediated Spin Beating in Electrostatically Bound Charge Carrier Pairs
journal, January 2010

  • McCamey, D. R.; van Schooten, K. J.; Baker, W. J.
  • Physical Review Letters, Vol. 104, Issue 1, Article No. 017601
  • DOI: 10.1103/PhysRevLett.104.017601

Vertical organic spin valves in perpendicular magnetic fields
journal, August 2013


Semiclassical description of electron spin motion in radicals including the effect of electron hopping
journal, April 1978

  • Schulten, Klaus; Wolynes, Peter G.
  • The Journal of Chemical Physics, Vol. 68, Issue 7
  • DOI: 10.1063/1.436135

Distinguishing Spin Relaxation Mechanisms in Organic Semiconductors
journal, April 2013


Hanle effect missing in a prototypical organic spintronic device
journal, March 2013

  • Riminucci, Alberto; Prezioso, Mirko; Pernechele, Chiara
  • Applied Physics Letters, Vol. 102, Issue 9
  • DOI: 10.1063/1.4794408

Room-temperature coupling between electrical current and nuclear spins in OLEDs
journal, September 2014


Organic spintronics
journal, June 2007

  • Naber, W. J. M.; Faez, S.; Wiel, W. G. van der
  • Journal of Physics D: Applied Physics, Vol. 40, Issue 12
  • DOI: 10.1088/0022-3727/40/12/R01

Electron spin relaxation by nuclei in semiconductor quantum dots
journal, April 2002


Spin-orbit coupling and its effects in organic solids
journal, March 2012


Random Walks on Lattices. II
journal, February 1965

  • Montroll, Elliott W.; Weiss, George H.
  • Journal of Mathematical Physics, Vol. 6, Issue 2
  • DOI: 10.1063/1.1704269

Solution of the time-dependent Schrödinger equation for two-dimensional spin-1/2 Heisenberg systems
journal, April 1993


Spin relaxation of a diffusively moving carrier in a random hyperfine field
journal, November 2014


Spin relaxation in materials lacking coherent charge transport
journal, September 2014


Evolution of localized electron spin in a nuclear spin environment
journal, November 2004