Arsenault Lab | Research Overview
Arsenault Lab | Research Overview
The dynamics of condensed phase systems are often governed by underlying heterarchical interactions. A key question lies in understanding how these interdependent couplings, manifesting across energetic and spatial scales, shape potential energy landscapes and give rise to function. These processes frequently unfold away from equilibrium and require highly sensitive experimental approaches capable of capturing their evolution in time. In the Arsenault Lab, we pursue this question by studying a broad set of systems using the tailored, time-resolved multidimensional spectroscopies we develop. These systems include macromolecules, materials, and other condensed phase platforms not typically explored within the same laboratory. Below, we outline several current challenges that motivate our work.
Macromolecular Design | We are interested in how proteins function as tunable nanoscale environments capable of directing energy and charge flow. This behavior underpins essential biological processes—such as light harvesting, enzymatic catalysis, and electron transport—and suggests new opportunities to harness proteins as customizable condensed phase scaffolds with functionality beyond that of individual molecules or systems defined by fixed intermolecular interactions. Yet this multiscale dynamic tuning, from local protein-cofactor interactions to collective intra- and inter-protein motions, forms a coupled network that poses a complex challenge to unravel. Our lab investigates these problems using original ultrafast spectroscopic methods designed to selectively and directly interrogate coupled vibrational and electronic dynamics in proteins and bio-inspired constructs. We are also interested in how insights into complex structure-dynamics relationships gained from our experiments can synergize with advances in protein engineering.
Quantum Matter | We are interested in how many-body correlation effects in quantum materials give rise to new phases of matter, exotic quasiparticles, and other strongly correlated states. Understanding these phenomena is essential for harnessing them in transformative quantum information and optoelectronic technologies. In many cases, our understanding of these emergent properties remains nascent, often relying on simplified model Hamiltonians that neglect couplings between distinct degrees of freedom. Our lab aims to bring a new perspective through ultrafast multidimensional experiments designed to directly probe and disentangle dynamic many-body interactions in designer crystals and van der Waals-based devices that are obscured or entirely inaccessible with other measurements. By bridging chemical and physical viewpoints, we also explore how local couplings and collective phenomena shape material behavior.
At a broad level, proteins and quantum materials both serve as structured playgrounds for energy and charge, albeit with distinct atomic architectures. A parallel interest of the Arsenault Lab is whether design principles can be meaningfully extrapolated across macromolecular and materials regimes.
Methods Innovations | Experimentally, studying complex and/or strongly interacting condensed phase systems poses a challenge: balancing a comprehensive view with specificity. To bridge this gap, our lab develops and applies multidimensional spectroscopies that employ tailored pulse sequences spanning from the UV to the THz. Untethered to any particular spectral region, these methods allow for the selective investigation of dynamic correlations between disparate degrees of freedom, distributed across energy and length scales. Beyond the specific applications described above, these methods are broadly applicable to a range of photochemical and photophysical questions (among others) throughout the condensed phase. We also explore many of these directions as part of our ongoing research.
Our experimental capabilities uniquely combine state-of-the-art multicolor generation and detection schemes. The variable-repetition-rate, few-femtosecond pulses driving these experiments are also frequently used to investigate systems at temperatures down to 4 K and with micron-scale spatial resolution.