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Article ; Online: Toward quantum sensing of chiral induced spin selectivity: Probing donor-bridge-acceptor molecules with NV centers in diamond.

Völker, Laura A / Herb, Konstantin / Janitz, Erika / Degen, Christian L / Abendroth, John M

2023 Volume 158, Issue 16

Abstract: Photoexcitable donor-bridge-acceptor (D-B-A) molecules that support intramolecular charge transfer are ideal platforms to probe the influence of chiral induced spin selectivity (CISS) in electron transfer and resulting radical pairs. In particular, the ... ...

Abstract	Photoexcitable donor-bridge-acceptor (D-B-A) molecules that support intramolecular charge transfer are ideal platforms to probe the influence of chiral induced spin selectivity (CISS) in electron transfer and resulting radical pairs. In particular, the extent to which CISS influences spin polarization or spin coherence in the initial state of spin-correlated radical pairs following charge transfer through a chiral bridge remains an open question. Here, we introduce a quantum sensing scheme to measure directly the hypothesized spin polarization in radical pairs using shallow nitrogen-vacancy (NV) centers in diamond at the single- to few-molecule level. Importantly, we highlight the perturbative nature of the electron spin-spin dipolar coupling within the radical pair and demonstrate how Lee-Goldburg decoupling can preserve spin polarization in D-B-A molecules for enantioselective detection by a single NV center. The proposed measurements will provide fresh insight into spin selectivity in electron transfer reactions.
Language	English
Publishing date	2023-04-21
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/5.0145466
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Multidimensional Spectroscopy of Nuclear Spin Clusters in Diamond.

Herb, Konstantin / Segawa, Takuya F / Völker, Laura A / Abendroth, John M / Janitz, Erika / Zhu, Tianqi / Degen, Christian L

Physical review letters

2024 Volume 132, Issue 13, Page(s) 133002

Abstract: Optically active spin defects in solids offer promising platforms to investigate nuclear spin clusters with high sensitivity and atomic-site resolution. To leverage near-surface defects for molecular structure analysis in chemical and biological contexts ...

Abstract	Optically active spin defects in solids offer promising platforms to investigate nuclear spin clusters with high sensitivity and atomic-site resolution. To leverage near-surface defects for molecular structure analysis in chemical and biological contexts using nuclear magnetic resonance (NMR), further advances in spectroscopic characterization of nuclear environments are essential. Here, we report Fourier spectroscopy techniques to improve localization and mapping of the test bed ^{13}C nuclear spin environment of individual, shallow nitrogen-vacancy centers at room temperature. We use multidimensional spectroscopy, well-known from classical NMR, in combination with weak measurements of single-nuclear-spin precession. We demonstrate two examples of multidimensional NMR: (i) improved nuclear spin localization by separate encoding of the two hyperfine components along spectral dimensions and (ii) spectral editing of nuclear-spin pairs, including measurement of internuclear coupling constants. Our work adds important tools for the spectroscopic analysis of molecular structures by single-spin probes.
Language	English
Publishing date	2024-04-13
Publishing country	United States
Document type	Journal Article
ZDB-ID	208853-8
ISSN	1079-7114 ; 0031-9007
ISSN (online)	1079-7114
ISSN	0031-9007
DOI	10.1103/PhysRevLett.132.133002
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Article ; Online: Divalent Cation Dependence Enhances Dopamine Aptamer Biosensing.

Nakatsuka, Nako / Abendroth, John M / Yang, Kyung-Ae / Andrews, Anne M

ACS applied materials & interfaces

2021 Volume 13, Issue 8, Page(s) 9425–9435

Abstract: Oligonucleotide receptors (aptamers), which change conformation upon target recognition, enable electronic biosensing under high ionic-strength conditions when coupled to field-effect transistors (FETs). Because highly negatively charged aptamer ... ...

Abstract	Oligonucleotide receptors (aptamers), which change conformation upon target recognition, enable electronic biosensing under high ionic-strength conditions when coupled to field-effect transistors (FETs). Because highly negatively charged aptamer backbones are influenced by ion content and concentration, biosensor performance and target sensitivities were evaluated under application conditions. For a recently identified dopamine aptamer, physiological concentrations of Mg
MeSH term(s)	Aptamers, Nucleotide/chemistry ; Benzothiazoles/chemistry ; Biosensing Techniques/instrumentation ; Biosensing Techniques/methods ; Calcium/chemistry ; Dopamine/analysis ; Dopamine/chemistry ; Electrochemical Techniques/instrumentation ; Electrochemical Techniques/methods ; G-Quadruplexes/drug effects ; Magnesium/chemistry ; Serotonin/analysis ; Serotonin/chemistry ; Transistors, Electronic
Chemical Substances	Aptamers, Nucleotide ; Benzothiazoles ; thioflavin T (2390-54-7) ; Serotonin (333DO1RDJY) ; Magnesium (I38ZP9992A) ; Calcium (SY7Q814VUP) ; Dopamine (VTD58H1Z2X)
Language	English
Publishing date	2021-01-07
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.0c17535
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Single-Nitrogen-Vacancy NMR of Amine-Functionalized Diamond Surfaces.

Abendroth, John M / Herb, Konstantin / Janitz, Erika / Zhu, Tianqi / Völker, Laura A / Degen, Christian L

Nano letters

2022 Volume 22, Issue 18, Page(s) 7294–7303

Abstract: Nuclear magnetic resonance (NMR) imaging with shallow nitrogen-vacancy (NV) centers in diamond offers an exciting route toward sensitive and localized chemical characterization at the nanoscale. Remarkable progress has been made to combat the degradation ...

Abstract	Nuclear magnetic resonance (NMR) imaging with shallow nitrogen-vacancy (NV) centers in diamond offers an exciting route toward sensitive and localized chemical characterization at the nanoscale. Remarkable progress has been made to combat the degradation in coherence time and stability suffered by near-surface NV centers using suitable chemical surface termination. However, approaches that also enable robust control over adsorbed molecule density, orientation, and binding configuration are needed. We demonstrate a diamond surface preparation for mixed nitrogen- and oxygen-termination that simultaneously improves NV center coherence times for <10 nm-deep emitters and enables direct and recyclable chemical functionalization via amine-reactive cross-linking. Using this approach, we probe single NV centers embedded in nanopillar waveguides to perform
MeSH term(s)	Amines ; Diamond/chemistry ; Magnetic Resonance Spectroscopy/methods ; Nitrogen/chemistry ; Oxygen
Chemical Substances	Amines ; Diamond (7782-40-3) ; Nitrogen (N762921K75) ; Oxygen (S88TT14065)
Language	English
Publishing date	2022-09-07
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1530-6992
ISSN (online)	1530-6992
DOI	10.1021/acs.nanolett.2c00533
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Diamond surface engineering for molecular sensing with nitrogen-vacancy centers.

Janitz, Erika / Herb, Konstantin / Völker, Laura A / Huxter, William S / Degen, Christian L / Abendroth, John M

Journal of materials chemistry. C

2022 Volume 10, Issue 37, Page(s) 13533–13569

Abstract: Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen-vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface defects ...

Abstract	Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen-vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface defects facilitate detection of the minute magnetic fields generated by nuclear or electron spins outside of the diamond crystal, such as those in chemisorbed and physisorbed molecules. However, the promise of NV centers is hindered by a severe degradation of critical sensor properties, namely charge stability and spin coherence, near surfaces (<
Language	English
Publishing date	2022-09-01
Publishing country	England
Document type	Journal Article ; Review
ZDB-ID	2702245-6
ISSN	2050-7534 ; 2050-7526
ISSN (online)	2050-7534
ISSN	2050-7526
DOI	10.1039/d2tc01258h
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Article ; Online: Spatial Correlation between Fluctuating and Static Fields over Metal and Dielectric Substrates.

Héritier, Martin / Pachlatko, Raphael / Tao, Ye / Abendroth, John M / Degen, Christian L / Eichler, Alexander

Physical review letters

2021 Volume 127, Issue 21, Page(s) 216101

Abstract: We report spatially resolved measurements of static and fluctuating electric fields over conductive (Au) and nonconductive (SiO_{2}) surfaces. Using an ultrasensitive "nanoladder" cantilever probe to scan over these surfaces at distances of a few tens of ...

Abstract	We report spatially resolved measurements of static and fluctuating electric fields over conductive (Au) and nonconductive (SiO_{2}) surfaces. Using an ultrasensitive "nanoladder" cantilever probe to scan over these surfaces at distances of a few tens of nanometers, we record changes in the probe resonance frequency and damping that we associate with static and fluctuating fields, respectively. We find static and fluctuating fields to be spatially correlated. Furthermore, the fields are of similar magnitude for the two materials. We quantitatively describe the observed effects on the basis of trapped surface charges and dielectric fluctuations in an adsorbate layer. Our results are consistent with organic adsorbates significantly contributing to surface dissipation that affects nanomechanical sensors, trapped ions, superconducting resonators, and color centers in diamond.
Language	English
Publishing date	2021-12-03
Publishing country	United States
Document type	Journal Article
ZDB-ID	208853-8
ISSN	1079-7114 ; 0031-9007
ISSN (online)	1079-7114
ISSN	0031-9007
DOI	10.1103/PhysRevLett.127.216101
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Article: Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces

Solomon, Michelle L / Abendroth, John M / Poulikakos, Lisa V / Hu, Jack / Dionne, Jennifer A

Journal of the American Chemical Society. 2020 Oct. 13, v. 142, no. 43

2020

Abstract: Strong enhancement of molecular circular dichroism (CD) has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study ... ...

Abstract	Strong enhancement of molecular circular dichroism (CD) has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost CD. We use fluorescence-detected circular dichroism (FDCD) spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk arrays. Importantly, the molecules and nanodisk antennas have spectrally coincident resonances, and our fluorescence technique allows us to deconvolute absorption in the nanodisks from the molecules. We find that enhanced FDCD signals depend on nanophotonic resonances, in good agreement with simulated differential absorption and optical chirality density, while no signal is detected from molecules adsorbed on featureless silicon surfaces. These results verify the potential of nanophotonic platforms to be used for asymmetric photolysis with lower energy requirements.
Keywords	absorption ; circular dichroism spectroscopy ; energy ; fluorescence ; optical isomerism ; photolysis ; silicon
Language	English
Dates of publication	2020-1013
Size	p. 18304-18309.
Publishing place	American Chemical Society
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c07140
Database	NAL-Catalogue (AGRICOLA)

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Book ; Online: Diamond surface engineering for molecular sensing with nitrogen-vacancy centers

Janitz, Erika / Herb, Konstantin / Völker, Laura A. / Huxter, William S. / Degen, Christian L. / Abendroth, John M.

2022

Abstract: Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen--vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface ... ...

Abstract	Quantum sensing using optically addressable atomic-scale defects, such as the nitrogen--vacancy (NV) center in diamond, provides new opportunities for sensitive and highly localized characterization of chemical functionality. Notably, near-surface defects facilitate detection of the minute magnetic fields generated by nuclear or electron spins outside of the diamond crystal, such as those in chemisorbed and physisorbed molecules. However, the promise of NV centers is hindered by a severe degradation of critical sensor properties, namely charge stability and spin coherence, near surfaces (< ca. 10 nm deep). Moreover, applications in the chemical sciences require methods for covalent bonding of target molecules to diamond with robust control over density, orientation, and binding configuration. This forward-looking Review provides a survey of the rapidly converging fields of diamond surface science and NV-center physics, highlighting their combined potential for quantum sensing of molecules. We outline the diamond surface properties that are advantageous for NV-sensing applications, and discuss strategies to mitigate deleterious effects while simultaneously providing avenues for chemical attachment. Finally, we present an outlook on emerging applications in which the unprecedented sensitivity and spatial resolution of NV-based sensing could provide unique insight into chemically functionalized surfaces at the single-molecule level. Comment: Review paper, 36 pages
Keywords	Condensed Matter - Materials Science ; Physics - Applied Physics ; Quantum Physics
Subject code	541
Publishing date	2022-07-15
Publishing country	us
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article ; Online: Rapid genetic screening with high quality factor metasurfaces.

Hu, Jack / Safir, Fareeha / Chang, Kai / Dagli, Sahil / Balch, Halleh B / Abendroth, John M / Dixon, Jefferson / Moradifar, Parivash / Dolia, Varun / Sahoo, Malaya K / Pinsky, Benjamin A / Jeffrey, Stefanie S / Lawrence, Mark / Dionne, Jennifer A

Nature communications

2023 Volume 14, Issue 1, Page(s) 4486

Abstract: Genetic analysis methods are foundational to advancing personalized medicine, accelerating disease diagnostics, and monitoring the health of organisms and ecosystems. Current nucleic acid technologies such as polymerase chain reaction (PCR) and next- ... ...

Abstract	Genetic analysis methods are foundational to advancing personalized medicine, accelerating disease diagnostics, and monitoring the health of organisms and ecosystems. Current nucleic acid technologies such as polymerase chain reaction (PCR) and next-generation sequencing (NGS) rely on sample amplification and can suffer from inhibition. Here, we introduce a label-free genetic screening platform based on high quality (high-Q) factor silicon nanoantennas functionalized with nucleic acid fragments. Each high-Q nanoantenna exhibits average resonant quality factors of 2,200 in physiological buffer. We quantitatively detect two gene fragments, SARS-CoV-2 envelope (E) and open reading frame 1b (ORF1b), with high-specificity via DNA hybridization. We also demonstrate femtomolar sensitivity in buffer and nanomolar sensitivity in spiked nasopharyngeal eluates within 5 minutes. Nanoantennas are patterned at densities of 160,000 devices per cm
MeSH term(s)	Humans ; SARS-CoV-2/genetics ; COVID-19/diagnosis ; COVID-19/genetics ; Ecosystem ; Genetic Testing ; Nucleic Acids ; Sensitivity and Specificity ; Nucleic Acid Amplification Techniques/methods
Chemical Substances	Nucleic Acids
Language	English
Publishing date	2023-07-26
Publishing country	England
Document type	Journal Article ; Research Support, N.I.H., Extramural ; Research Support, U.S. Gov't, Non-P.H.S. ; Research Support, Non-U.S. Gov't
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-023-39721-w
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Fluorescence-Detected Circular Dichroism of a Chiral Molecular Monolayer with Dielectric Metasurfaces.

Solomon, Michelle L / Abendroth, John M / Poulikakos, Lisa V / Hu, Jack / Dionne, Jennifer A

Journal of the American Chemical Society

2020 Volume 142, Issue 43, Page(s) 18304–18309

Abstract	Strong enhancement of molecular circular dichroism (CD) has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost CD. We use fluorescence-detected circular dichroism (FDCD) spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk arrays. Importantly, the molecules and nanodisk antennas have spectrally coincident resonances, and our fluorescence technique allows us to deconvolute absorption in the nanodisks from the molecules. We find that enhanced FDCD signals depend on nanophotonic resonances, in good agreement with simulated differential absorption and optical chirality density, while no signal is detected from molecules adsorbed on featureless silicon surfaces. These results verify the potential of nanophotonic platforms to be used for asymmetric photolysis with lower energy requirements.
Language	English
Publishing date	2020-10-13
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.0c07140
Database	MEDical Literature Analysis and Retrieval System OnLINE

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