Daniel G. Oblinsky
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View article: Red-Light-Induced Ligand-to-Metal Charge Transfer Catalysis by Tuning the Axial Coordination of Cobyrinate
Red-Light-Induced Ligand-to-Metal Charge Transfer Catalysis by Tuning the Axial Coordination of Cobyrinate Open
Photoinduced ligand-to-metal charge transfer (LMCT) is a powerful technique for the formation of reactive radical species via homolytic cleavage of the metal-ligand bond. Here, we present that the excited state LMCT of a cobyrinate complex…
View article: Engineering a Photoenzyme to Use Red Light
Engineering a Photoenzyme to Use Red Light Open
Photoenzymatic catalysis is an emerging platform for asymmetric synthesis. In most of these reactions, the protein templates a charge transfer complex between the cofactor and substrate, which absorbs in the blue region of the electromagne…
View article: Mechanism and Dynamics of Photodecarboxylation Catalyzed by Lactate Monooxygenase
Mechanism and Dynamics of Photodecarboxylation Catalyzed by Lactate Monooxygenase Open
Photoenzymes are a rare class of biocatalysts that use light to facilitate chemical reactions. Many of these catalysts utilize a flavin cofactor to absorb light, suggesting that other flavoproteins might have latent photochemical functions…
View article: Regioselective Radical Alkylation of Arenes Using Evolved Photoenzymes
Regioselective Radical Alkylation of Arenes Using Evolved Photoenzymes Open
Substituted arenes are ubiquitous in molecules with medicinal functions, making their synthesis a critical consideration when designing synthetic routes. Regioselective C-H functionalization reactions are attractive for preparing alkylated…
View article: Regioselective Radical Alkylation of Arenes Using Evolved Photoenzymes
Regioselective Radical Alkylation of Arenes Using Evolved Photoenzymes Open
Substituted arenes are ubiquitous in molecules with medicinal functions, making their synthesis a critical consideration when designing synthetic routes. 1,2 Regioselective C–H functionalization reactions are attractive for preparing alkyl…
View article: Electronic Energy Migration in Microtubules
Electronic Energy Migration in Microtubules Open
The repeating arrangement of tubulin dimers confers great mechanical strength to microtubules, which are used as scaffolds for intracellular macromolecular transport in cells and exploited in biohybrid devices. The crystalline order in a m…
View article: A telecom O-band emitter in diamond
A telecom O-band emitter in diamond Open
Color centers in diamond are promising platforms for quantum technologies. Most color centers in diamond discovered thus far emit in the visible or near-infrared wavelength range, which are incompatible with long-distance fiber communicati…
View article: Electronic Energy Migration in Microtubules
Electronic Energy Migration in Microtubules Open
The repeating arrangement of tubulin dimers confers great mechanical strength to microtubules, which are used as scaffolds for intracellular macromolecular transport in cells and exploited in biohybrid devices. The crystalline order in a m…
View article: Radius measurement via super-resolution microscopy enables the development of a variable radii proximity labeling platform
Radius measurement via super-resolution microscopy enables the development of a variable radii proximity labeling platform Open
The elucidation of protein interaction networks is critical to understanding fundamental biology as well as developing new therapeutics. Proximity labeling platforms (PLPs) are state-of-the-art technologies that enable the discovery and de…
View article: Radical Termination via β-Scission Enables Photoenzymatic Allylic Alkylation Using “Ene”-Reductases
Radical Termination via β-Scission Enables Photoenzymatic Allylic Alkylation Using “Ene”-Reductases Open
Allylations are practical transformations that forge C–C bonds while introducing an alkene for further chemical manipulations. Here, we report a photoenzymatic allylation of α-chloroamides with allyl silanes using flavin-dependent ‘ene’-re…
View article: μMap-Red: Proximity Labeling by Red Light Photocatalysis
μMap-Red: Proximity Labeling by Red Light Photocatalysis Open
Modern proximity labeling techniques have enabled significant advances in understanding biomolecular interactions. However, current tools primarily utilize activation modes that are incompatible with complex biological environments, limiti…
View article: Using Enzymes to Tame Nitrogen-Centered Radicals for Enantioselective Hydroamination
Using Enzymes to Tame Nitrogen-Centered Radicals for Enantioselective Hydroamination Open
The construction of C–N bonds is essential for the preparation of numerous molecules critical to modern society1,2. Nature has evolved enzymes to facilitate these transformations using nucleophilic and nitrene transfer mechanisms3,4. Howev…
View article: Engineering a Non‐Natural Photoenzyme for Improved Photon Efficiency**
Engineering a Non‐Natural Photoenzyme for Improved Photon Efficiency** Open
Photoenzymes are biological catalysts that use light to convert starting materials into products. These catalysts require photon absorption for each turnover, making quantum efficiency an important optimization parameter. Flavin‐dependent …
View article: Engineering a Non‐Natural Photoenzyme for Improved Photon Efficiency**
Engineering a Non‐Natural Photoenzyme for Improved Photon Efficiency** Open
Photoenzymes are biological catalysts that use light to convert starting materials into products. These catalysts require photon absorption for each turnover, making quantum efficiency an important optimization parameter. Flavin‐dependent …
View article: Spectroscopic and Photophysical Investigation of Model Dipyrroles Common to Bilins: Exploring Natural Design for Steering Torsion to Divergent Functions
Spectroscopic and Photophysical Investigation of Model Dipyrroles Common to Bilins: Exploring Natural Design for Steering Torsion to Divergent Functions Open
Biliproteins are a unique class of photosynthetic proteins in their diverse, and at times, divergent biophysical function. The two contexts of photosynthetic light harvesting and photoreception demonstrate characteristically opposite crite…
View article: Photoenzymatic Reductions Enabled by Direct Excitation of Flavin-Dependent “Ene”-Reductases
Photoenzymatic Reductions Enabled by Direct Excitation of Flavin-Dependent “Ene”-Reductases Open
Non-natural photoenzymatic reactions reported to date have depended on the excitation of electron donor-acceptor complexes formed between substrates and cofactors within protein active sites to facilitate electron transfer. While this mech…
View article: Quaternary Charge-Transfer Complex Enables Photoenzymatic Intermolecular Hydroalkylation of Olefins
Quaternary Charge-Transfer Complex Enables Photoenzymatic Intermolecular Hydroalkylation of Olefins Open
Intermolecular C-C bond-forming reactions are underdeveloped transformations in the field of biocatalysis. Here we report a photoenzymatic intermolecular hydroalkylation of olefins catalyzed by flavin-dependent 'ene'-reductases. Radical in…
View article: Active-Site Environmental Factors Customize the Photophysics of Photoenzymatic Old Yellow Enzymes
Active-Site Environmental Factors Customize the Photophysics of Photoenzymatic Old Yellow Enzymes Open
The development of non-natural photoenzymatic systems has reinvigorated the study of photoinduced electron transfer (ET) within protein active sites, providing new and unique platforms for understanding how biological environments affect p…
View article: Quaternary Charge-Transfer Complex Enables Photoenzymatic In-termolecular Hydroalkylation of Olefins
Quaternary Charge-Transfer Complex Enables Photoenzymatic In-termolecular Hydroalkylation of Olefins Open
Intermolecular C–C bond-forming reactions are underdeveloped transformations in the field of biocatalysis. Here we report a photoenzymatic intermolecular hydroalkylation of olefins catalyzed by flavin-dependent ‘ene’reductases. Radical ini…
View article: Quaternary Charge-Transfer Complex Enables Photoenzymatic In-termolecular Hydroalkylation of Olefins
Quaternary Charge-Transfer Complex Enables Photoenzymatic In-termolecular Hydroalkylation of Olefins Open
Intermolecular C–C bond-forming reactions are underdeveloped transformations in the field of biocatalysis. Here we report a photoenzymatic intermolecular hydroalkylation of olefins catalyzed by flavin-dependent ‘ene’reductases. Radical ini…
View article: Ring currents modulate optoelectronic properties of aromatic chromophores at 25 T
Ring currents modulate optoelectronic properties of aromatic chromophores at 25 T Open
Significance Applying magnetic fields is a powerful strategy to study the electronic properties of inorganic materials and paramagnetic organic systems due to their straightforward Zeeman interactions. We demonstrate with magnetic fields a…
View article: Asymmetric Redox-Neutral Radical Cyclization Catalyzed by Flavin-Dependent ‘Ene’-Reductases
Asymmetric Redox-Neutral Radical Cyclization Catalyzed by Flavin-Dependent ‘Ene’-Reductases Open
Flavin-dependent ‘ene’-reductases (EREDs) are exquisite catalysts for effecting stereoselective reductions. While these reactions typically proceed through a hydride transfer mechanism, we recently found that EREDs can also catalyze reduct…