Award Abstract # 1903839
Collaborative Research - GOALI: Dynamic Nuclear Spin Hyperpolarization via Color Centers in Diamond

NSF Org: CHE
Division Of Chemistry
Recipient: RESEARCH FOUNDATION OF THE CITY UNIVERSITY OF NEW YORK
Initial Amendment Date: July 19, 2019
Latest Amendment Date: July 15, 2020
Award Number: 1903839
Award Instrument: Standard Grant
Program Manager: Kelsey Cook
CHE
 Division Of Chemistry
MPS
 Directorate for Mathematical and Physical Sciences
Start Date: August 1, 2019
End Date: July 31, 2022 (Estimated)
Total Intended Award Amount: $314,324.00
Total Awarded Amount to Date: $361,324.00
Funds Obligated to Date: FY 2019 = $314,324.00
FY 2020 = $47,000.00
History of Investigator:
  • Carlos Meriles (Principal Investigator)
    cmeriles@ccny.cuny.edu
  • Joseph Tabeling (Co-Principal Investigator)
Recipient Sponsored Research Office: CUNY City College
160 CONVENT AVE
NEW YORK
NY  US  10031-9101
(212)650-5418
Sponsor Congressional District: 13
Primary Place of Performance: CUNY-City College of New York
160 Convent Ave, Marshak Rm 419
New York
NY  US  10031-9101
Primary Place of Performance
Congressional District:
13
Unique Entity Identifier (UEI): L952KGDMSLV5
Parent UEI:
NSF Program(s): OFFICE OF MULTIDISCIPLINARY AC,
EPMD-ElectrnPhoton&MagnDevices,
Chemical Measurement & Imaging,
QIS - Quantum Information Scie
Primary Program Source: 01001920DB NSF RESEARCH & RELATED ACTIVIT
01002021DB NSF RESEARCH & RELATED ACTIVIT
Program Reference Code(s): 1504, 7203, 7237
Program Element Code(s): 125300, 151700, 688000, 728100
Award Agency Code: 4900
Fund Agency Code: 4900
Assistance Listing Number(s): 47.049

ABSTRACT

With support from the Chemical Measurement and Imaging Program, Professors Carlos A. Meriles (City College of New York) and Jeffrey A. Reimer (University of California at Berkeley), in collaboration with Delaware Diamond Knives, are working to enhance the sensitivity of nuclear magnetic resonance (NMR), an important chemical analysis tool used for wide-ranging applications that include determination of protein structure and folding dynamics; medical imaging (MRI); and probing porous rocks in search of oil. For all such applications, the limited sensitivity of NMR imposes restrictions on the minimum amount of sample that can be detected, and can result in long measurement times and limited access to expensive instrumentation. The Meriles/Reimer team is studying and utilizing interactions between light and engineered diamond crystals to enhance the sensitivity of NMR by several orders of magnitude under ambient conditions. Their multi-pronged approach - combining both fundamental and applied science - is enabling a wider range of applications and development of new contrast agents for multi-modal in-vivo imaging. This multi-institutional project is providing training opportunities targeting a diverse STEM workforce, including a number of educational opportunities at the undergraduate and high-school levels.

The Meriles and Reimer groups are pursuing a novel route to generating augmented nuclear spin polarization by leveraging the singular properties of nitrogen-vacancy (NV) centers, a paramagnetic defect in diamond that can be completely polarized via optical excitation under ambient conditions. Specific aims include (i) defect engineering in diamond and systematic characterization of nuclear polarization buildup; (ii) development of novel, enhanced spin polarization transfer schemes tailored to both single-crystal and powdered diamond; and (iii) proof-of-principle demonstrations of polarization transfer from diamond to solid and fluid targets. The approach employs low magnetic fields (~10 mT), ambient (or near-ambient) temperature, and mild optical excitation, circumventing the need for complex, expensive hardware while offering regimes of spin polarization dynamics not explored in the past. The partnership with Delaware Diamond Knives is providing access to a broad set of diamond samples, whose characteristics (nitrogen content, 13C enrichment, surface termination, single crystal or variable-particle-size powder, etc.) are specifically tailored to attain optimal polarization transfer. The work aims to enable studies of molecular moieties in trace concentrations (typical in biochemistry), investigation of mass-limited systems (often found in synthetic chemistry), and high-throughput characterization of molecular libraries (as required in the pharmaceutical industry).

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

PUBLICATIONS PRODUCED AS A RESULT OF THIS RESEARCH

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A. Ajoy, A. Sarkar "Low-field microwave-mediated hyperpolarization in optically pumped diamond" Journal of magnetic resonance , v.331 , 2022 https://doi.org/10.1016/j.jmr.2021.107021 Citation Details
Ajoy, A. and Nazaryan, R. and Druga, E. and Liu, K. and Aguilar, A. and Han, B. and Gierth, M. and Oon, J. T. and Safvati, B. and Tsang, R. and Walton, J. H. and Suter, D. and Meriles, C. A. and Reimer, J. A. and Pines, A. "Room temperature optical nanodiamond hyperpolarizer : Physics, design, and operation" Review of Scientific Instruments , v.91 , 2020 https://doi.org/10.1063/1.5131655 Citation Details
Henshaw, Jacob and Pagliero, Daniela and Zangara, Pablo R. and Franzoni, María B. and Ajoy, Ashok and Acosta, Rodolfo H. and Reimer, Jeffrey A. and Pines, Alexander and Meriles, Carlos A. "Carbon-13 dynamic nuclear polarization in diamond via a microwave-free integrated cross effect" Proceedings of the National Academy of Sciences , v.116 , 2019 10.1073/pnas.1908780116 Citation Details
Lv, Xudong and Walton, Jeffrey H. and Druga, Emanuel and Wang, Fei and Aguilar, Alessandra and McKnelly, Tommy and Nazaryan, Raffi and Liu, Fanglin Linda and Wu, Lan and Shenderova, Olga and Vigneron, Daniel B. and Meriles, Carlos A. and Reimer, Jeffrey A "Background-free dual-mode optical and 13 C magnetic resonance imaging in diamond particles" Proceedings of the National Academy of Sciences , v.118 , 2021 https://doi.org/10.1073/pnas.2023579118 Citation Details
Pagliero, Daniela and Zangara, Pablo R. and Henshaw, Jacob and Ajoy, Ashok and Acosta, Rodolfo H. and Manson, Neil and Reimer, Jeffrey A. and Pines, Alexander and Meriles, Carlos A. "Magnetic field induced delocalization in hybrid electron-nuclear spin ensembles" Physical Review B , v.103 , 2021 https://doi.org/10.1103/PhysRevB.103.064310 Citation Details
Pagliero, Daniela and Zangara, Pablo R. and Henshaw, Jacob and Ajoy, Ashok and Acosta, Rodolfo H. and Reimer, Jeffrey A. and Pines, Alexander and Meriles, Carlos A. "Optically pumped spin polarization as a probe of many-body thermalization" Science Advances , v.6 , 2020 https://doi.org/10.1126/sciadv.aaz6986 Citation Details
Zangara, Pablo R. and Pagliero, Daniela and Ajoy, Ashok and Acosta, Rodolfo H. and Reimer, Jeffrey A. and Meriles, Carlos A. "Nuclear spin temperature reversal via continuous radio-frequency driving" Physical Review B , v.103 , 2021 https://doi.org/10.1103/PhysRevB.103.085205 Citation Details
Zangara, Pablo R. and Wood, Alexander W. and Doherty, Marcus A. and Meriles, Carlos "Mechanical rotation via optical pumping of paramagnetic impurities" Physical Review B , v.100 , 2019 10.1103/PhysRevB.100.235410 Citation Details

PROJECT OUTCOMES REPORT

Disclaimer

This Project Outcomes Report for the General Public is displayed verbatim as submitted by the Principal Investigator (PI) for this award. Any opinions, findings, and conclusions or recommendations expressed in this Report are those of the PI and do not necessarily reflect the views of the National Science Foundation; NSF has not approved or endorsed its content.

Nuclear Magnetic Resonance (NMR) is a widely used spectroscopic and imaging technique with a range of applications in medical diagnosis, biochemical studies, and analytical science. Key to any NMR measurement is the sample?s ?nuclear spin polarization?, which is a measure of the fractional alignment of the atomic magnetic moments towards a preferential direction. Typical NMR devices impart polarization through the use of strong magnetic fields, which, unfortunately, is largely inefficient. Dynamic nuclear polarization (DNP) methods have been introduced in the past to circumvent this problem but those in use today typically rely on paramagnetic molecules dissolved in a solid matrix and require high-frequency microwave excitation as well as extreme cryogenic temperatures.

Throughout the award, we examined a novel route to generating augmented nuclear spin polarization by leveraging on the singular properties of the so-called nitrogen-vacancy (NV) center, a paramagnetic defect in diamond that can be completely polarized via optical excitation under ambient conditions. This effort brought together groups at the City College of New York, the University of California at Berkeley and collaborators at Delaware Diamond Knives, along with several other academic and industrial partners, both domestic and international. Some of the key outcomes of the project include:

  • A deeper understanding of the physical mechanisms underpinning the generation of bulk nuclear polarization in a solid.
  • A battery of novel nuclear spin polarization strategies adapted to single crystal and powder geometries.
  • New diamond processing schemes, including flash high-temperature annealing protocols.
  • Innovative instrumentation for the investigation and deployment of dynamic nuclear polarization at low magnetic fields.
  • A range of novel applications in other related study areas, e.g., in the form of dual imaging modalities combining optical microscopy and magnetic resonance, novel NV-assisted nanoscale sensing schemes, and alternative DNP routes that do not require the use of microwave or optical excitation.

In total, our research led to 12 scientific papers, several of which have been published in high-impact international journals; it also resulted in multiple conference presentations and seminars as well as three patent applications, one of which has already been issued. Accompanying this effort, the present project served as a platform to train students at all levels (from high school, to undergrad, to masters, to graduates) as well as several postdocs. This work is significant in that many of these students belong to under-represented groups or are first generation college students. Finally, this project helped develop various institutional resources, e.g., in the form of new curricula, remote access resources, and online educational material for the general public.  

 


Last Modified: 11/28/2022
Modified by: Carlos A Meriles

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