Department of Chemistry

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David Waldeck

Professor

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G-10 CHVRN
Chevron Science Center, 219 Parkman Avenue

Pittsburgh, PA 15260
412-624-8430

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Research Overview

Professor Waldeck's research program uses methods of spectroscopy, electrochemistry, and microscopy to examine the nature of the Chiral-Induced Spin Selectivity (CISS) effect and to explore ways in which it can be exploited technologically. First discovered in 1999, CISS refers to the preference for a chiral molecule or chiral material to preferentially transmit electrons of one spin orientation over that of the other. This spin-filtering of electron currents has important implications for electron transfer and electrochemical processes.  In addition to spin-filtered currents, charge displacement currents in chiral molecules are spin-polarized, and this has important implications for enantioselective intermolecular interactions.

The Waldeck Lab is currently accepting new graduate students.

 

Chiral Nanomaterials

The Waldeck group is exploring design features of chiral symmetry that promote the efficient flow of electron charge and electron spin in nanoparticle-based materials which form by self-assembly. Chiral molecules and nanostructures manifest unusual electronic and magnetic properties; for example, chiral materials are able to filter electron spins. These recent findings establish new opportunities across a range of applications in optically coupled electronic devices, electronic devices whose function is derived from the spin of electrons, and devices that are important in quantum information science.  The Waldeck group is elucidating how a chiral nanostructured material’s architecture and optical properties may be designed to promote efficient charge and spin transport - properties that are essential for developing efficient energy conversion and optoelectronic devices.

 

Electrochemistry

Waldeck’s group explores the use of spin-polarized electrons to improve the chemical selectivity, and energy efficiency, in electrocatalysis. By building on ideas from the CISS effect, they are developing new electrode materials and electrode designs for generating spin polarized electrons and evaluating their performance as electrocatalysts. The idea that chiral catalysts and chiral electrodes can be used to generate spin polarized electron currents which can then be used to promote particular chemical reaction pathways represents a fundamentally new approach for electrocatalysis and electrosynthesis. Their recent work on the oxygen evolution reaction, which is critically important for energy technologies, shows that chiral electrocatalysts can be used to improve the faradaic efficiency of electrochemical reactions that involve the generation of high spin products, i.e., triplet oxygen.

 

Enantioselectivity and Homochirality

The Waldeck group is exploring how the homochirality of biological molecules (oligopeptides, proteins, and nucleic acids) and of molecular assemblies affect electron transfer, enantioselective molecular recognition, and biological allostery. Conventional wisdom considers that enantiospecific interactions between molecules is dominated by stereoisomeric effects, however recent work shows that spin polarization of chiral molecules can be comparable to stereoisomeric effects.  Moreover, protein voltammetry studies show that electron transfer through homochiral assemblies is more efficient than that through heterochiral assemblies. Given the ubiquitous homochirality of living organisms, the connection between the electron spin and chirality holds important implications for biochemical and biological processes.

Awards

  • Fellow of the American Chemical Society, 2020
  • ISE Bioelectrochemistry Prize, 2018
  • American Association for the Advancement of Science Fellow, 2017
  • ACS-WCC Award for Encouraging Women in Chemistry 2016
  • ACS Pittsburgh Award 2014
  • Fellow of the American Physical Society, 2005
  • Belkin Visiting Professor, Weizmann Institute 1998 - 1999
  • Chancellor's Distinguished Research Award, University of Pittsburgh, 1994

Publications

“Chiral Induced Spin Selectivity,” B.P. Bloom*, Y. Paltiel*, R. Naaman*, D.H. Waldeck* Chem. Rev. 2024
“Electron-donating functional groups strengthen ligand-induced chiral imprinting on CsPbBr3 quantum dots,” W.A. Dunlap-Shohl, N. Tabassum, P. Zhang, E. Shiby, D.N. Beratan, D.H. Waldeck Sci Rep 2024, 14, 336
“Spin polarized electron dynamics enhance water splitting efficiency by yttrium iron garnet photoanodes: a new platform for spin selective photocatalysis,” H. Gajapathy, S. Bandaranayake, E. Hruska, A. Vadakkayil, B.P. Bloom, S. Londo, J. McClellan, J. Guo, D. Russell, F.M.F. de Groot, F. Yang, D.H. Waldeck, M. Schultze, L.R. Baker* Chem. Sci. 2024, Advance Article
“On the circularly polarized luminescence of individual triplet sublevels,” C. Climent, E.J. Schelter, D.H. Waldeck, S.A. Vinogradov, J.E. Subotnik J. Chem. Phys. 2023, 159, 134304
“Tailored PVDF Graft Copolymers via ATRP as High-Performance NCM811 Cathode Binders,” T. Liu, R. Parekh, Piotr, B.P. Bloom, Y. Zhao, S.Y. An, B. Pan, R. Yin, D.H. Waldeck, J.F. Whitacre*, K. Matyjaszewski ACS Materials Lett. 2023, 5, 2594-2603
“Beyond Stereoisomeric Effects: Exploring the Importance of Intermolecular Electron Spin Interactions in Biorecognition,” Y. Lu, M. Joy, B.P. Bloom, D.H. Waldeck* J. Phys. Chem. Lett. 2023, 14, 7032-7037
“Examining the Effects of Homochirality for Electron Transfer in Protein Assemblies,” J. Wei, B.P. Bloom, W.A. Dunlap-Shohl, C.B. Clever, J.E. Rivas, D.H. Waldeck* J. Phys. Chem. B 2023, 127, 6462-6469
“Spin-Based Chiral Separations and the Importance of Molecule–Solvent Interactions,” Y. Lu, T, Qiu, B.P. Bloom, J.E. Subotnik, D.H. Waldeck* J. Phys. Chem. C 2023, 127, 14155-14162
“Spin Selectivity Damage Dependence of Adsorption of dsDNA on Ferromagnets,” K. Santra, Y. Lu, D.H. Waldeck*, R. Naaman* J. Phys. Chem. B 2023, 127, 2344-2350
“Size-dependent chiro-optical properties of CsPbBr3 nanoparticles,” N. Tabassum, Z.N. Georgieva, G.H. Debnath, D.H. Waldeck* Nanoscale 2023, 15, 2143-2151
“New Perspective on Electron Transfer through Molecules,” R. Naaman*, D.H. Waldeck, J. Fransson J. Phys. Chem. Lett. 2022, 13, 11753-11759
“Benchmarking Chiral Induced Spin Selectivity Measurements - Towards Meaningful Comparisons of Chiral Biomolecule Spin Polarizations,” C. Clever, E. Wierzbinski, B.P. Bloom, Y. Lu, H.M. Grimm, S.R. Rao, W.S. Horne, D.H. Waldeck Irs. J. Chem. 2022, 62, e202200045
“Homochirality and chiral-induced spin selectivity: A new spin on the origin of life,” B.P. Bloom, A.R. Waldeck, D.H. Waldeck PNAS 2022, 119, e2210505119
“Ligand Coverage and Exciton Delocalization Control Chiral Imprinting in Perovskite Nanoplatelets,” Z.N. Georgieva, Z. Zhang, P. Zhang, B.P. Bloom, D.N. Beratan*, D.H. Waldeck* J. Phys. Chem. C 2022, 126, 15986-15995
“Spin-Polarized Photoemission from Chiral CuO Catalyst Thin Films,” P.V. Möllers*, J. Wei, S. Salamon, M. Bartsch, H. Wende, D.H. Waldeck, H. Zacharias* ACS Nano 2022, 16, 12145-112455
“Chirality enhances oxygen reduction,” Y. Sang, F. Tassinari, K. Santra, W. Zhang, C. Fontanesi, B.P. Bloom, D.H. Waldeck, J. Fransson, R. Naaman PNAS 2022, 119, e2202650119
“Evaluating Inter-Lanthanide Interactions in Co-Doped Zinc Sulfide Nanoparticles for Multiplex Assays,” S. Rudra, G.H. Debnath, N. Bhunia, B.P. Bloom, D.H. Waldeck*, P. Mukerjee* J. Phys. Chem. C 2022, 126, 11723-11734
“Electron transfer and spin–orbit coupling: Can nuclear motion lead to spin selective rates?,” S.S. Chandran, Y. Wu, H. Teh, D.H. Waldeck, J.E. Subotnik J. Chem. Phys. 2022, 156, 174113
“Room temperature doping of Ln3+ in perovskite nanoparticles: a halide exchange mediated cation exchange approach,” G.H. Debnath, B.P. Bloom, S. Tan, D.H. Waldeck* Nanoscale 2022, 14, 6037-6051
“Polymer-Stabilized Liquid Metal Nanoparticles as a Scalable Current Collector Engineering Approach Enabling Lithium Metal Anodes,” T. Liu, X. Wu, S. Zhu, F. Lorandi, L. Ni, S. Li, M. Sun, B.P. Bloom, D.H. Waldeck, V. Viswanathan*, J.F. Whitacre*, K. Matyjaszewski* ACS Appl. Energy Mater. 2022, 5, 3615-3625
“A Chirality-Based Quantum Leap,” C.D. Aiello*, J.M. Abendroth*, M. Abbas, A. Afanasev, S. Agarwal, A.S. Banerjee, D.N. Beratan, J.N. Belling, B. Berche, A. Botana, J.R. Caram, G.L. Celardo, G. Cuniberti, A. Garcia-Etzarri, A. Dianat, I. Diez-Perez, Y. Guo, R. Gutierrez, C. Herrmann, J. Hihath, S. Kale, P. Kurian, Y. Lai, T. Liu, A. Lopez, E. Medina, V. Mujica, R. Naaman, M. Noormandipour, J.L. Palma, Y. Paltiel, W. Petuskey, J.C. Ribeiro-Silva, J.J. Saenz, E.J.G. Santos, M. Solyanik-Gorgone, V.J. Sorger, D.M. Stemer, J.M. Ugalde, A. Valdes-Curiel, S. Varela, D.H. Waldeck, M.R. Wasielewski, P.S. Weiss, H. Zacharias, Q.H. Wang* ACS Nano 2022, 4989-5035
“Theory of Chirality Induced Spin Selectivity: Progress and Challenges,” F. Evers, A. Aharony, N. Bar-Gill, O. Entin-Wohlman, P. Hedegård, O. Hod, P. Jelinek, G. Kamieniarz, M. Lemeshko, K. Michaeli, V. Mujica, R. Naaman, Y. Paltiel, S. Refaely-Abramson, O. Tal, J. Thijssen, M. Thoss, J.M. van Ruitenbeek, L. Venkataraman, D.H. Waldeck, B. Yan, L. Kronik Adv. Mater. 2022, 34, 2106629
“Chiral Induced Spin Selectivity and Its Implications for Biological Functions,” R. Naaman, Y. Paltiel, D.H. Waldeck Annu Rev Biophys 2022, 55, 99-114