Research in the Hadt laboratory is broadly based in physical inorganic chemistry.
We employ air- and moisture-free synthetic techniques, computational analysis, and a wide range of steady state and time-resolved spectroscopies spanning many orders of magnitude in photon energy to understand the roles of transition metal electronic structure across interdisciplinary areas of chemistry, biology, and physics.
Two areas of research interest include:
Photocatalysis. Understanding geometric and electronic structure contributions to ground and excited state first-row transition metal catalyzed cross-coupling reactions
Spin Dynamics. Connecting molecular electronic structure and electron spin decoherence mechanisms for quantum information science (QIS)
Photocatalysis. Cross-coupling reactions enable the construction of new C–X bonds (X = C, N, O, etc.) necessary for the synthesis of existing pharmaceuticals and new drug candidates. While precious metal Pd-based catalysts are largely used on an industrial scale, the combination of the disparate electron transfer properties of earth abundant first-row transition metal catalysts and the possibility of harnessing light energy to generate uniquely reactive electronic states represents an attractive, sustainable approach to accessing new mechanistic possibilities for drug synthesis and discovery.
We use a combination of synthetic, spectroscopic, and computational approaches to define the critical electronic structure contributions to ground-state Cu- and Ni-catalyzed cross-couplings. Furthermore, we use and develop time-resolved spectroscopies to elucidate key excited state factors that allow for sustainable light-driven syntheses.
Molecular Spin Dynamics. The next generation of information processing devices will rely upon detailed understanding of quantum phenomena at the single atom and molecule level. We are developing a new approach rooted in molecular structure to understand electron spin relaxation mechanisms that lead to the destruction of quantum information, particularly at higher temperatures.
To do this, we employ and develop new lines of spectroscopic inquiry to evaluate critical spin-phonon coupling processes that control high temperature quantum coherence/decoherence. More generally, we seek to tie together new experimental and theoretical approaches to study the structural and dynamic electronic properties of molecular systems for QIS.
Biological Quantum Sensing. Building on the previous goal, we also seek to develop and apply molecular QIS concepts to the biophysics domain. In molecular QIS, the focus has been on understanding intramolecular vs intermolecular contributions to decoherence properties of quantum bit (qubit) candidates. We seek to incorporate molecular qubits into biological macromolecules to enable controllable, fundamental studies of molecular coherence properties across a range of biochemical microenvironments and interfaces.
As part of this, we seek to develop a reciprocal relationship between quantum biology and molecular QIS that will not only develop quantum sensors (qusors) for biological applications but will also improve understanding of quantum processes needed for applications of molecular QIS in technological devices.
Example Spectroscopic and Computational Techniques
- Steady State Electronic Absorption and Fluorescence
- Circular Dichroism (CD) and Variable-Temperature Variable-Field (VTVH) Magnetic Circular Dichroism (MCD)
- Circularly Polarized Luminescence (CPL) and Magnetic Circular Polarized Luminescence (MCPL)
- Resonance Raman (rR)
- Electron Paramagnetic Resonance (EPR)
- X-ray Absorption and Emission (XAS/XES)
- Resonant Inelastic X-ray Scattering (RIXS)
- Transient Optical Absorption and Emission
- Transient XAS/XES
- Time-Resolved Kerr and Faraday Rotation
- Density Functional Theory (DFT) and Time-Dependent DFT (TDDFT)
- Ab initio methods (CASSCF/QD-NEVPT2)