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Novel methods in solid- and liquid-state NMR spectroscopy: (A, B, E) investigation of internal dynamics in proteins; (C, D) enhancement of sensitivity by dynamic nuclear polarization.

Applicant Bodenhausen Geoffrey
Number 134771
Funding scheme Project funding (Div. I-III)
Research institution Laboratoire de résonance magnétique biomoléculaire EPFL - SB - ISIC - LRMB
Institution of higher education EPF Lausanne - EPFL
Main discipline Physical Chemistry
Start/End 01.04.2011 - 31.03.2013
Approved amount 473'323.00
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Keywords (8)

Dynamic Nuclear Polarization (DNP); Dissolution DNP in liquids; Slow dynamic processes in proteins; Long-lived spin states in liquids; ‘In situ' DNP in solids; DNP-enhanced surface NMR; Fast correlated dynamics in proteins; Nitrogen-14 Solid-State NMR

Lay Summary (English)

Lead
Lay summary

slow dynamic processesNuclear Magnetic Resonance (NMR)spectroscopy is a formidable tool for the investigation of matter in numerousdisciplines of science. Long-lived states will allow us to characterize therates of of suchas folding/unfolding of proteins. in biomolecules. fast correlated processesDouble resonance methods will give access to Dynamic Nuclear Polarization (DNP) . surface chemistrywill beused to investigate the largely unexplored field of DNPwill also be exploited to study slow processes in solution, such as diffusionand metabolic reactions. 

Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Analysis of sensitivity enhancement by dynamic nuclear polarization in solid-state NMR: a case study of functionalized mesoporous materials.
Kobayashi Takeshi, Lafon Olivier, Thankamony Aany S Lilly, Slowing Igor I, Kandel Kapil, Carnevale Diego, Vitzthum Veronika, Vezin Hervé, Amoureux Jean-Paul, Bodenhausen Geoffrey, Pruski Marek (2013), Analysis of sensitivity enhancement by dynamic nuclear polarization in solid-state NMR: a case study of functionalized mesoporous materials., in Physical chemistry chemical physics : PCCP, 15(15), 5553-62.
Mesoporous silica nanoparticles loaded with surfactant: Low temperature magic angle spinning 13C and 29Si NMR enhanced by dynamic nuclear polarization
Lafon O, Thankamony ASL, Kobayashi T, Carnevale D, Vitzthum V, Slowing II, Kandel K, Vezin H, Amoureux J-P, Bodenhausen G, Pruski M (2013), Mesoporous silica nanoparticles loaded with surfactant: Low temperature magic angle spinning 13C and 29Si NMR enhanced by dynamic nuclear polarization, in Journal of Physical Chemistry C, 117(3), 1375-1382.
How to tickle spins with a fourier transform NMR spectrometer
Segawa TF, Carnevale D, Bodenhausen G (2013), How to tickle spins with a fourier transform NMR spectrometer, in ChemPhysChem, 14(2), 369-373.
Boosting dissolution dynamic nuclear polarization by cross polarization
Bornet A, Melzi R, Perez Linde AJ, Hautle P, Van Den Brandt B, Jannin S, Bodenhausen G (2013), Boosting dissolution dynamic nuclear polarization by cross polarization, in Journal of Physical Chemistry Letters, 4(1), 111-114.
Dynamic Nuclear Polarization and other magnetic ideas at EPFL
Bornet A, Milani J, Wang S, Mammoli D, Buratto R, Salvi N, Segawa TF, Vitzthum V, Miéville P, Srichinthalapalli N, Perez-Linde AJ, Carnevale D, Jannin S, Caporini M, Ulzega S, Rey M, Bodenhausen G (2012), Dynamic Nuclear Polarization and other magnetic ideas at EPFL, in Chimia, 66(10), 734-740.
High field dynamic nuclear polarization at 6.7 T: Carbon-13 polarization above 70% within 20 min
Jannin S, Bornet A, Melzi R, Bodenhausen G (2012), High field dynamic nuclear polarization at 6.7 T: Carbon-13 polarization above 70% within 20 min, in Chemical Physics Letters, 549, 99-102.
Uniform broadband excitation of crystallites in rotating solids using interleaved sequences of delays alternating with nutation
Vitzthum V, Caporini MA, Ulzega S, Trébosc J, Lafon O, Amoureux J-P, Bodenhausen G (2012), Uniform broadband excitation of crystallites in rotating solids using interleaved sequences of delays alternating with nutation, in Journal of Magnetic Resonance, 223, 228-236.
Efficient determination of diffusion coefficients by monitoring transport during recovery delays in NMR
Augustyniak Rafal, Ferrage Fabien, Damblon Christian, Bodenhausen Geoffrey, Pelupessy Philippe (2012), Efficient determination of diffusion coefficients by monitoring transport during recovery delays in NMR, in CHEMICAL COMMUNICATIONS, 48(43), 5307-5309.
Broadband excitation in solid-state NMR of paramagnetic samples using Delays Alternating with Nutation for Tailored Excitation ('Para-DANTE')
Carnevale Diego, Vitzthum Veronika, Lafon Olivier, Trebosc Julien, Amoureux Jean-Paul, Bodenhausen Geoffrey (2012), Broadband excitation in solid-state NMR of paramagnetic samples using Delays Alternating with Nutation for Tailored Excitation ('Para-DANTE'), in CHEMICAL PHYSICS LETTERS, 553, 68-76.
Polychromatic Decoupling of a Manifold of Homonuclear Scalar Interactions in Solution-State NMR
Carnevale Diego, Segawa Takuya F., Bodenhausen Geoffrey (2012), Polychromatic Decoupling of a Manifold of Homonuclear Scalar Interactions in Solution-State NMR, in CHEMISTRY-A EUROPEAN JOURNAL, 18(37), 11573-11576.
Cross Polarization for Dissolution Dynamic Nuclear Polarization Experiments at Readily Accessible Temperatures 1.2 < T < 4.2 K
Bornet Aurelien, Melzi Roberto, Jannin Sami, Bodenhausen Geoffrey (2012), Cross Polarization for Dissolution Dynamic Nuclear Polarization Experiments at Readily Accessible Temperatures 1.2 < T < 4.2 K, in APPLIED MAGNETIC RESONANCE, 43(1-2), 107-117.
Ultrahigh-resolution magnetic resonance in inhomogeneous magnetic fields: two-dimensional long-lived-coherence correlation spectroscopy.
Chinthalapalli Srinivas, Bornet Aurélien, Segawa Takuya F, Sarkar Riddhiman, Jannin Sami, Bodenhausen Geoffrey (2012), Ultrahigh-resolution magnetic resonance in inhomogeneous magnetic fields: two-dimensional long-lived-coherence correlation spectroscopy., in Physical review letters, 109(4), 047602-047602.
Boosting the Sensitivity of Ligand-Protein Screening by NMR of Long-Lived States
Salvi N, Buratto R, Bornet A, Ulzega S, Rebollo IR, Angelini A, Heinis C, Bodenhausen G (2012), Boosting the Sensitivity of Ligand-Protein Screening by NMR of Long-Lived States, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134(27), 11076-11079.
Insights into internal dynamics of 6-phosphogluconolactonase from Trypanosoma brucei studied by nuclear magnetic resonance and molecular dynamics.
Calligari Paolo A, Salgado Gilmar F, Pelupessy Philippe, Lopes Philippe, Ouazzani Jamal, Bodenhausen Geoffrey, Abergel Daniel (2012), Insights into internal dynamics of 6-phosphogluconolactonase from Trypanosoma brucei studied by nuclear magnetic resonance and molecular dynamics., in Proteins, 80(4), 1196-210.
Transverse Relaxation of Scalar Coupled Protons in Magnetic Resonance of Non-Deuterated Proteins
Segawa TF, Baishya B, Bodenhausen G (2012), Transverse Relaxation of Scalar Coupled Protons in Magnetic Resonance of Non-Deuterated Proteins, in APPLIED MAGNETIC RESONANCE, 42(3), 353-361.
Composite pulses for efficient excitation of half-integer quadrupolar nuclei in NMR of static and spinning solid samples
Carnevale D, Bodenhausen G (2012), Composite pulses for efficient excitation of half-integer quadrupolar nuclei in NMR of static and spinning solid samples, in CHEMICAL PHYSICS LETTERS, 530, 120-125.
Dynamic nuclear polarization of quadrupolar nuclei using cross polarization from protons: surface-enhanced aluminium-27 NMR.
Vitzthum Veronika, Miéville Pascal, Carnevale Diego, Caporini Marc A, Gajan David, Copéret Christophe, Lelli Moreno, Zagdoun Alexandre, Rossini Aaron J, Lesage Anne, Emsley Lyndon, Bodenhausen Geoffrey (2012), Dynamic nuclear polarization of quadrupolar nuclei using cross polarization from protons: surface-enhanced aluminium-27 NMR., in Chemical communications (Cambridge, England), 48(14), 1988-90.
Time Scales of Slow Motions in Ubiquitin Explored by Heteronuclear Double Resonance
Salvi N, Ulzega S, Ferrage F, Bodenhausen G (2012), Time Scales of Slow Motions in Ubiquitin Explored by Heteronuclear Double Resonance, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 134(5), 2481-2484.
Spin echo NMR spectra without J modulation
Aguilar JA, Nilsson M, Bodenhausen G, Morris GA (2012), Spin echo NMR spectra without J modulation, in CHEMICAL COMMUNICATIONS, 48(6), 811-813.
1H, 13C and 15N resonance assignment of a 114-residue fragment of Engrailed 2 homeoprotein, a partially disordered protein.
Augustyniak R, Balayssac S, Ferrage F, Bodenhausen G, Lequin O (2011), 1H, 13C and 15N resonance assignment of a 114-residue fragment of Engrailed 2 homeoprotein, a partially disordered protein., in Biomolecular NMR assignments, 5(2), 229-231.
Reflections of pathways: A short perspective on 'Selection of coherence transfer pathways in NMR pulse experiments
Bodenhausen G (2011), Reflections of pathways: A short perspective on 'Selection of coherence transfer pathways in NMR pulse experiments, in Journal of Magnetic Resonance, 213(2), 295-297.
Extending Timescales and Narrowing Linewidths in NMR
Segawa TF, Bornet A, Salvi N, Mieville P, Vitzthum V, Carnevale D, Jannin S, Caporini MA, Ulzega S, Vasos PR, Rey M, Bodenhausen G (2011), Extending Timescales and Narrowing Linewidths in NMR, in CHIMIA, 65(9), 652-655.
NMR of Insensitive Nuclei Enhanced by Dynamic Nuclear Polarization
Mieville P, Jannin S, Helm L, Bodenhausen G (2011), NMR of Insensitive Nuclei Enhanced by Dynamic Nuclear Polarization, in CHIMIA, 65(4), 260-263.
Disentangling Crystallographic Inequivalence and Crystallographic Forms of L-Arginine by One- and Two-Dimensional Solid-State NMR Spectroscopy
Herbert-Pucheta JE, Colaux H, Bodenhausen G, Tekely P (2011), Disentangling Crystallographic Inequivalence and Crystallographic Forms of L-Arginine by One- and Two-Dimensional Solid-State NMR Spectroscopy, in JOURNAL OF PHYSICAL CHEMISTRY B, 115(51), 15415-15421.
Low-temperature cross polarization in view of enhancing dissolution Dynamic Nuclear Polarization in NMR
Jannin S, Bornet A, Colombo S, Bodenhausen G (2011), Low-temperature cross polarization in view of enhancing dissolution Dynamic Nuclear Polarization in NMR, in CHEMICAL PHYSICS LETTERS, 517(4-6), 234-236.
A spinning thermometer to monitor microwave heating and glass transitions in dynamic nuclear polarization
Mieville P, Vitzthum V, Caporini MA, Jannin S, Gerber-Lemaire S, Bodenhausen G (2011), A spinning thermometer to monitor microwave heating and glass transitions in dynamic nuclear polarization, in MAGNETIC RESONANCE IN CHEMISTRY, 49(11), 689-692.
Fractional Spin-Labeling of Polymers for Enhancing NMR Sensitivity by Solvent-Free Dynamic Nuclear Polarization
Vitzthum V, Borcard F, Jannin S, Morin M, Mieville P, Caporini MA, Sienkiewicz A, Gerber-Lemaire S, Bodenhausen G (2011), Fractional Spin-Labeling of Polymers for Enhancing NMR Sensitivity by Solvent-Free Dynamic Nuclear Polarization, in CHEMPHYSCHEM, 12(16), 2929-2932.
Long-Lived States to Monitor Protein Unfolding by Proton NMR
Bornet A, Ahuja P, Sarkar R, Fernandes L, Hadji S, Lee SY, Haririnia A, Fushman D, Bodenhausen G, Vasos PR (2011), Long-Lived States to Monitor Protein Unfolding by Proton NMR, in CHEMPHYSCHEM, 12(15), 2729-2734.
Ultra High-Resolution NMR: Sustained Induction Decays of Long-Lived Coherences
Bornet A, Jannin S, Konter JA, Hautle P, van den Brandt B, Bodenhausen G (2011), Ultra High-Resolution NMR: Sustained Induction Decays of Long-Lived Coherences, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 133(39), 15644-15649.
Broadband excitation and indirect detection of nitrogen-14 in rotating solids using Delays Alternating with Nutation (DANTE)
Vitzthum V, Caporini MA, Ulzega S, Bodenhausen G (2011), Broadband excitation and indirect detection of nitrogen-14 in rotating solids using Delays Alternating with Nutation (DANTE), in JOURNAL OF MAGNETIC RESONANCE, 212(1), 234-239.
Quenching homonuclear couplings in magnetic resonance by trains of non-refocusing pulses
Baishya B, Segawa TF, Bodenhausen G (2011), Quenching homonuclear couplings in magnetic resonance by trains of non-refocusing pulses, in JOURNAL OF MAGNETIC RESONANCE, 211(2), 240-242.
Three-field NMR to preserve hyperpolarized proton magnetization as long-lived states in moderate magnetic fields
Bornet A, Jannin S, Bodenhausen G (2011), Three-field NMR to preserve hyperpolarized proton magnetization as long-lived states in moderate magnetic fields, in CHEMICAL PHYSICS LETTERS, 512(4-6), 151-154.
Efficiency at high spinning frequencies of heteronuclear decoupling methods designed to quench rotary resonance
Weingarth M, Trebosc J, Amoureux JP, Bodenhausen G, Tekely P (2011), Efficiency at high spinning frequencies of heteronuclear decoupling methods designed to quench rotary resonance, in SOLID STATE NUCLEAR MAGNETIC RESONANCE, 40(1), 21-26.
Long-lived coherences for line-narrowing in high-field NMR
Sarkar R, Ahuja P, Vasos PR, Bornet A, Wagnieres O, Bodenhausen G (2011), Long-lived coherences for line-narrowing in high-field NMR, in PROGRESS IN NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY, 59(1), 83-90.
Methods to determine slow diffusion coefficients of biomolecules. Applications to Engrailed 2, a partially disordered protein
Augustyniak R, Ferrage F, Paquin R, Lequin O, Bodenhausen G (2011), Methods to determine slow diffusion coefficients of biomolecules. Applications to Engrailed 2, a partially disordered protein, in JOURNAL OF BIOMOLECULAR NMR, 50(3), 209-218.
Sensitive (13)C- (13)C correlation spectra of amyloid fibrils at very high spinning frequencies and magnetic fields.
Weingarth Markus, Masuda Yuichi, Takegoshi K, Bodenhausen Geoffrey, Tekely Piotr (2011), Sensitive (13)C- (13)C correlation spectra of amyloid fibrils at very high spinning frequencies and magnetic fields., in Journal of biomolecular NMR, 50(2), 129-36.
Relaxometry of insensitive nuclei: Optimizing dissolution dynamic nuclear polarization
Mieville P, Jannin S, Bodenhausen G (2011), Relaxometry of insensitive nuclei: Optimizing dissolution dynamic nuclear polarization, in JOURNAL OF MAGNETIC RESONANCE, 210(1), 137-140.
Fast Characterization of Functionalized Silica Materials by Silicon-29 Surface-Enhanced NMR Spectroscopy Using Dynamic Nuclear Polarization
Lelli M, Gajan D, Lesage A, Caporini MA, Vitzthum V, Mieville P, Heroguel F, Rascon F, Roussey A, Thieuleux C, Boualleg M, Veyre L, Bodenhausen G, Coperet C, Emsley L (2011), Fast Characterization of Functionalized Silica Materials by Silicon-29 Surface-Enhanced NMR Spectroscopy Using Dynamic Nuclear Polarization, in JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 133(7), 2104-2107.
Control of Cross Relaxation of Multiple-Quantum Coherences Induced by Fast Chemical Exchange under Heteronuclear Double-Resonance Irradiation
Ulzega S, Salvi N, Segawa TF, Ferrage F, Bodenhausen G (2011), Control of Cross Relaxation of Multiple-Quantum Coherences Induced by Fast Chemical Exchange under Heteronuclear Double-Resonance Irradiation, in CHEMPHYSCHEM, 12(2), 333-341.

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
EUROMAR 2012 01.07.2012 DUBLIN
Board of editors, Progress in NMR Spectroscopy 01.01.2012 London
EUROMAR 21.08.2011 Frankfurt


Knowledge transfer events

Active participation

Title Type of contribution Date Place Persons involved
52nd ENC Conference 10.04.2011 ASILOMAR, USA


Communication with the public

Communication Title Media Place Year
Talks/events/exhibitions RMN International

Associated projects

Number Title Start Funding scheme
124694 Methods for enhancing sensitivity and magnetisation lifetimes in liquid- and solid-state NMR 01.04.2009 Project funding (Div. I-III)
124694 Methods for enhancing sensitivity and magnetisation lifetimes in liquid- and solid-state NMR 01.04.2009 Project funding (Div. I-III)
146380 Methods for MRI, solid- and liquid-state NMR spectroscopy 01.04.2013 Project funding (Div. I-III)

Abstract

Nuclear Magnetic Resonance (NMR) spectroscopy is a formidable tool for the investigation of matter through the measurement of nuclear spin interactions that has virtually infinite applications in numerous disciplines of science. This research plan is based on five subprojects. (A) Long-Lived States (LLS’s) of nuclear spins exhibit lifetimes that can be much longer than the spin-lattice relaxation time T1 (TLLS >> T1) and thus represent extremely interesting probes for slow dynamic processes. We will develop methods to excite and sustain LLS’s in proteins and access dynamics such as folding/unfolding processes in complex biomolecules. We also plan to search for LLS’s in water molecules and possibly exploit them to study slow processes such as hindered diffusion and metabolic chemical reactions. (B) We have recently developed new Heteronuclear Double Resonance (HDR) methods that give us access to fast correlated processes in biomolecules. These methods will offer a unique insight into dynamic modes that extend over contiguous regions of a protein structure. They could also be extended to nucleic acids (e.g., RNA). (C) Dynamic Nuclear Polarization (DNP) has the potential of enhancing NMR signals by several orders of magnitude by coupling nuclear spins to the large reservoir of electrons. A solid-state DNP - NMR system (in-situ DNP) has been recently installed at EPFL and will be used to investigate the largely unexplored field of surface chemistry. Surface science is a very active research area for technological innovations that can boast a number of Nobel Prizes in chemistry and significant financial investments. (D) In liquids, we have successfully applied Dissolution-DNP to various nuclei and developed novel challenging methods. We have shown that hyperpolarized magnetization can be stored in long-lived nuclear spin states (DNP - LLS). This method will be further developed and exploited to study slow processes, such as diffusion phenomena and metabolic reactions. We will also carry out further work on scavenging of free radicals, relaxometry, proton DNP and DNP of macromolecules. (E) Our lab, a worldwide leader in solid-state 14N NMR spectroscopy, will be soon (2011) equipped with a probe for fast (up to 70 kHz) magic angle spinning (MAS). This will boost our efforts directed to enhance the efficiency of our solid-state methods, with a special focus on the investigation of fast local dynamics.
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