University Professor, Chemistry and Physics, University of Toronto; Co-founding director of Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany; Director of Max Planck Group at Centre for Free Electron Laser Science/DESY, University of Hamburg; Distinguished Research Faculty Chair in Chemical and Biological Physics; Fellow of the Royal Society; Fellow of the Royal Society of Canada; Fellow of the Chemical Institute of Canada; Fellow of the Optical Society of America; Fellow of the Royal Society of Chemistry
Degrees / Research Training
1983-1984 NATO Science Fellow, Université Joseph Fourier, Dr. P.Trommsdorff
1978-1983 Stanford University, Ph.D., 1983, Advisor: Professor Michael D. Fayer
1974-1978 University of Manitoba, B.Sc. Honours, 1978, Advisor: Professor Bryan R. Henry
2007-present, University Professor, Chemistry and Physics, University of Toronto
2014-2020, Co-Founding Director, Max Planck Institute for the Structure and Dynamics of Matter
2010-2014, Director, Max Planck Group, Centre for Free Electron Laser Science/DESY, University of Hamburg
2005-2010, Director of the Institute for Optical Sciences, University of Toronto
1995-present, Professor of Chemistry and Physics, University of Toronto
1992-1995, Professor of Chemistry and Optics, University of Rochester
1988-1992, Associate Professor of Chemistry and Optics, University of Rochester
1984-1988, Assistant Professor of Chemistry, University of Rochester
Relevant Annotated Publications 2017-2023 re. Current Research Activities
"Quantum coherent energy transport in the Fenna–Matthews–Olson complex at low temperature” by H. -G. Duan et al. R. J. Dwayne Miller, PNAS, Vol 119, No. 49 e2212630119 (2022). Issues of Quantum Biology and prospect for nature exploiting quantum phase relationships to direct biological processes was put to rest with this paper. The long-held speculation of coherent energy transport for photosynthetic systems was finally observed, where there is a clear signature. The onset of coherent transport only occurred below 20K. The detailed T dependence of transport determined the system-bath coupling parameters to establish that biological systems, even for the fastest process, are in the strong system-bath coupling limit. Nature rather than trying to exploit exotic quantum effects exploits dissipation via site energy engineering to unerringly direct energy over long length scales at the lowest possible energy losses to ensure directionality. The present work has determined the operating physics responsible for the apparent long-range correlations and high quantum efficiency (re-establishing a general principle in how biological systems are evolutionarily optimized.)
“Torsionally broken symmetry assists infrared excitation of biomimetic charge-coupled nuclear motions in the electronic ground state” G. Chatterjee..et al. R. J. Dwayne Miller, Chem. Sci., 2022, 13, 9392. This work was the first direct observation of a vibrational mode strongly modulating electronic surfaces by exploiting the same bond elongation (with charge displacement) as exploited by the primary step in vision. This new insight shows how to identify reactive modes without having to do any chemistry and opens up a new mechanism for control of ground state chemistry.
“Picosecond Infrared Laser Driven Sample Delivery for Simultaneous Liquid-phase and Gas-phase Electron Diffraction Studies”, by Z. Huang …R. J. Dwayne Miller, Structural Dynamics, 9, 054301 (2022). This work makes it possible to generate nanodroplets (liquid) and isolated gas phase molecules simultaneously, spatially separated in the plume expansion. This new experimental concept allows a direct observation of the difference of chemical dynamics with and without solvent in a single experiment. This work opens up the long held objective of physical chemistry to resolve the effect of the solvent coordinate on reactions – where most chemistry occurs.
“Disentangling surface atomic motions from surface field effects in ultrafast low-energy electron diffraction (LEED)” by C. Lee, A. Marx, G. Kassier, and R. J. Dwayne Miller, Comm. Materials, (2022) 3:10, doi.org/10.1038/s43246-022-00231-9, www.nature.com. This paper was able to quantify photoinduced emission processes that have hampered the use of LEED to study surface reaction dyamics. One of the most important chemical processes is heterogeneous catalysis. The paper now enables the direct observation of atomic motions during barrier crossing – the key process in catalysis.
“Quantum state tomography of molecules by ultrafast diffraction.” by M. Zhang….R. J. Dwayne Miller, and Zheng Li, Nature Communications 12, 5441 (2021). This paper solves the dimension problem in inverting diffraction results to probability distributions or wavefunctions. This work was based on ideas germinated in the development of an rf streak camera concept to separate electronic and nuclear distributions to unmask the forces leading to the key reaction modes directing chemistry – that make chemistry a transferrable concept. Theory work led by Zheng Li.
“Serial Electron Diffraction Data Processing With diffractem and CrystFEL”, by R. Bücker, P. Hogan-Lamarre, and R. J. Dwayne Miller, Frontiers in Molecular Biosciences Vol 8 (624264) 2021. One of the major problems in diffraction is indexing and it was not at all clear that given the extremely flat Ewald sphere (small scattering angles) for electron diffraction that it would be possible to find a general solution to uniquely index crystals as an essential step in the workflow for atomically resolved structures. This problem has been solved as outlined in this work. It is noteworthy that only nanograms of material are needed (nanocrystals) for electron diffraction/structure determination. This work holds promise to enable orders of reduction in material needs for chemical synthesis to move chemistry to true lab on a chip, and orders of magnitude higher throughput. This concept is being actively explored.
“Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite”, by H.-G. Duane, et al RJDM, JACS. DOI:10.1021/jacs.0c03970
(2020). This concept is being promoted as the next generation solar cell concept (cost/performance beyond Si). We discovered the mechanism responsible for the exceptionally high conversion efficiencies for this material. The issue has been stability. Photostability problem has been solved (now >10,000 hour lifetimes) re: physics to avoid interfacial recombination/degradation.
“Serial femtosecond and serial synchrotron crystallography can yield data of equivalent quality: a systematic comparison”, by P. Mehrabi, et al. R. J. Dwayne Miller Science Advances 2021; 7 : eabf1380. The chip concept developed by the group opens up serial sampling methods for microfocus x-ray beamlines to reduce x-ray radiation damage by spreading the dose over thousands of crystals. This approach provides similar, even superior, structural resolution (more stable, broader band source) than XFELs. This work opens up a much larger number of sources, over limited beam access at XFELs, for structure determination without limitations due to radiation damage. See work on serial nanoelectron diffraction as well.
“Utilizing relativistic time dilation for time-resolved studies” H. Daoud, and R. D. Dwayne Miller, The Journal of Chemical Physics 154, 111107 (2021). Work describes explicit use of relativistic reference frame to slow down time to observe fastest possible motions. (HZ student initiated).
“Compact Ho:YLF-pumped ZnGeP2-based optical parametric amplifiers tunable in the molecular fingerprint regime”, by S. Cheng, G. Chatterjee, F. Tellkamp, T. Lang, A. Ruehl, I. Hartl, and R. J. Dwayne Miller, Optics Letters Vol. 45, No. 8 (2020). After several years work, the IR Death Laser has been been realized. This source has sufficient pulse energy over a broad enough spectral range to do strong field control on the ground state to drive chemical processes (laser system not moved to Toronto).
“Intermolecular vibrations mediate ultrafast singlet fission”, by H. -G., Duan, A. Jha, X. Li, V. Tiwari, H. Ye, H., P. Nayak, X.-L Zhu, Z. Li, T. Martinez, M. Thorwart, and R. J. Dwayne Miller, Science Advances. (2020); 6 : eabb0052. Per title, a correlated lattice effect was found to strongly modulate the intersystem crossing process involved in singlet fission to provide new insight into factors controlling spin states.
“Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite” H.-G. Duane, V. Tiwari, A. Jha, G. Berdiyorov, A. Akimov, O. Vendrell, P. Mayak, H. Snaith, M. Thorwart, Z. Li, Z. M. Madjet, and R. J. Dwayne Miller. Journal of the American Chemical Society. DOI:10.1021/jacs.0c03970 (2020). This work provided a direct observation of the lattice coupling involved in charge transfer in these systems relevant to their high efficiency in charge transfer/solar energy conversion applications.
2019 – 2020
“Direct observation of nuclear reorganization driven by ultrafast spin transitions” by Y. Jiang, L. C. Liu, A. Sarracini, K. M. Krawczyk, J. S. Wentzell, C. Lu, E. L. Field, S. F. Matar, W. Gawelda, H. M. Müller-Werkmeister, R. J. Dwayne Miller. Nature Communications. 11(1530): 1-8 (2020). Spin transitions lead to changes in electron distribution viz Hund’s rule, a purely relativistic effect associated with electron motion that affects e-e correlations. A very simple concept was formulated to find key rxn modes to the spin induced change in e distribution. This work resolved the reduction of a 50+ dimensional problem reduce to just 4 key reaction modes – Hund’s rule in action.
“Mapping Atomic Motions with Electrons: Toward the Quantum Limit to Imaging Chemistry”, by Z. Li, S. Gyawali, A. A. Ischenko, S. A. Hayes, and R. J. Dwayne. Miller, ACS Photonics. 7(2): 296–320 (2020). This perspective article highlights the achievement of the fundamental space-time limit to imaging chemistry within the standard classical depiction of structures used in chemistry. This paper places a challenge to solve the quantum tomography problem to enable imaging time dependent wavefunctions and points out the physics to solve the dimension problem.
“Quantum Biology Revisited”, by J. Cao, R.J. Cogdel, D. F. Coker, H-G. Duan, J. Hauer, U. Kleinekathöfer, T. L. C. Jansen, T. Maňcal, R. J. D. Miller,* J. P. Ogilvie, V. I. Prokhorenko, T. Renger, H-S.Tan, R. Tempelaar, M. Thorwart, E. Thyrhaug, S. Westenhoff and D. Zigmantas, Science Advances. 6(14): EAAZ4888 (2020). This effort took over 3 years of constant meetings to properly describe energy transport in photosynthesis and put science right. The field of Quantum Biology emerged from an assertion that long lived beats observed in 2D data illustrated energy transport, the primary step in photosynthesis, involved wave-like or coherent motion, i.e., nature had discovered a design principle to beat quantum decoherence even in wet complex disordered media. The topic became highly popularized with new experiments and theory supporting the notion of Quantum Biology with over 5000 citations without critical evaluation of the concept. This paper (subjected to 20 reviewers in total) rigorously shows from both theory and experiment that the foundational work on this topic were based on a vibrational artifact. Rather than avoid dissipation that leads to decoherence, nature engineers site energies to exploit dissipation to yield downhill directed processes. The real marvel of nature is that she exploits this simple concept over all length and times scales – even the fastest biological processes of energy transport.
“Serial protein crystallography in an electron microscope”, by R. Bücker, P. Hogan-Lamarre, P. Mehrabi, E.-C. Schulz, L. Bultema, Y. Gevorkov, W. Brehm, O. Yefanov, D. Oberthür, G. Kassier, R. J. Dwayne Miller. Nature Communications. 11(996): 1-8 (2020). This new concept is equivalent to a table top $1B XFEL with the advantage of only requiring nanograms of material to determine structures. This development could change how chemistry and structural biology are done with respect to throughput and amount of needed precious material.
“Time-resolved crystallography reveals allosteric communication aligned with molecular breathing” by, P. Mehrabi, E.-C. Schulz, R. Dsouza, H. Müller-Werkmeister, F. Tellkamp, R. J. Dwayne Miller, E. F. Pai. Science. 365(6458): 1167–1170 (2019). This work was done in collaboration with Emil Pai. It is the first fully resolved enzymatic cycle. We discovered an unusual new mechanism of allosteric control that is clocked by periodic conformational motions.
“Liquid application method for time resolved analyses by serial synchrotron crystallography” P. Mehrabi, E.-C. Schulz, M. Agthe, S. Horrell, G. Bourenkov, D. von Stetten, J.-P. Leimkohl, H. Schikora, T. R. Schneider, A. R. Pearson, F. Tellkamp, R. J. Dwayne Miller. (2019). Nature Methods. 16(10): 979–982 (2019). This work now opens up atomically resolved dynamics for all enzymatic systems, requiring micron crystals.
2018 – 2019
“Ultrafast dissolution and creation of bonds in IrTe2 induced by photodoping”, by S. I. Idetal, D. Zhang, A. Dijkstra, S. Artyukhin, S. Keskin, R. Cingolani, T. Shimojima, K. Ishizaka, H. Ishii, K. Kudao…R. J. Dwayune Miller, Science Advances 4 (7), eaar3867 (2018). This work was able to observe ultrafast bond formation due solely to electron correlation effects. To watch bond dissociation is relatively uneventful as it is driven entropically by coupling to continuum states. How can one get bond formation in this sea of possible motions? It was a remarkable effect.
“New frontiers in drug development utilizing desorption by impulsive vibrational excitation for sample preparation, tissue imaging and beyond”, W. Robertson, H. Schlüter, R J. Dwayne Miller, Q. C. Ji, Bioanalysis 10 (20), pp. 1625 - 1630 (2018). This paper highlights the enormous promise of PIRL-DIVE-MS to enable a frozen snapshot of tissue proteomes for quantifying disease states and detection of disease at the earliest possible stage. Ji is with Bristol Myer Squibb and is pushing for adoption in the pharma sector.
“The hit-and-return system enables efficient time-resolved serial synchrotron crystallography” E. -C. Schultz, et al. RJDM.. Nature methods 15 (11), pp. 901 - 904 (2018). This paper represents a major advance in technology for atomically resolved structural dynamics to resolve the full enzymatic cycle for the first time, discovering a conformational allosteric effect. The full molecular movie, published in Science, gives witness to an enzyme breaking the strongest single bond (C-F) in chemistry.
“Fabrication and characterization of a focused ion beam milled lanthanum hexaboride based cold field electron emitter source”, by G. Singh, R. Buecker , G. Kassier, M. Barthelmess, F. Zheng, V. Migunov, M. Kruth, R. E. Dunin Borkowski, S. T. Purcell, and R. J. Dwayne Miller, Applied Physics Letters 113 (9), 093101 (2018). This paper announces a simple method to reach the highest possible brightness for electron sources – sufficient brightness for real space imaging single molecule motions (e.g. DNA unwinding, Ribosome/RNA translation) at the atomic level – equivalent to a cold field emission gun (FEG) but able to with stand much higher current and normal HV rather than UHV as needed for cold FEGs.
“Optical fiber-driven low energy electron gun for ultrafast streak diffraction” by C. Lee, G. Kassier, and R. J. Dwayne Miller, Applied Physics Letters 113 (13), 133502 (2018). The group has finally opened up surface reactions to atomic inspection. Other groups have shown femtosecond LEED sources with few electrons. This approach is effectively orders of magnitude brighter with respect to image reconstruction. The design involves a simple fibre input and a photocapacitor. Its simplicity is its most important feature. It is smaller than a coffee cup.
2017 – 2018
“Nature Does Not Rely on Long-Lived Electronic Quantum Coherence for Photosynthetic Energy Transfer” by H.-G. Duan, V. I. Prokhorenko, R. J. Cogdell, K. Ashraf, A. L. Stevens, M. Thorwart, R. J. Dwayne Miller, Proceedings of the National Academy of Sciences 114 (32), pp. 8493–8498 (2017). This paper redid the key experiment for the Fenna Matthews Olsen (FMO complex under actual physiological conditions to show that the “signature” assigned to long lived electronic coherence was incorrectly assigned. The experiment was complemented by state-of-the art theory using explicitly the measured spectral density of state of the photosynthetic system (FMO). We and other groups have now done several systems clearly showing ultrafast electronic decoherence is too fast to support quantum coherence in directing energy transport. Nature explicity controls energy transport in photosynthesis by site energy engineering. Nature takes advantage of dissipation - not avoid it - to direct energy transport. This paper was the first of many to challenge the original work that launched Quantum Biology.
“Soft Picosecond Infrared Laser Extraction of Highly Charged Proteins and Peptides from Bulk Liquid Water for Mass Spectrometry” by Lu, Y; Pieters, L.; Robertson, W. D.; Miller, R. J. Dwayne, Analytical Chemistry 90, pp. 4422-4428 (2018). Picosecond Infrared Laser (PIRL) Technology – Major Advance in Medicine. This work established PIRL-DIVE-MS as having attomole sensitivity and with previous demonstration of proving a frozen snapshot of protein signatures and paved the way to molecular signatures of disease. Surgeons now have a veritable molecular bar code to guide surgery.
“Picosecond Infrared Laser (PIRL) application in stapes surgery – first experience in human temporal bones” by H. Petersen, A. Gliese, Y. Stober, S. Maier, N.-O. Hansen, S. Kruber, D. Eggert, M. Tóth, T. Gosau, H. Schlüter, K. Püschel, U. Schumacher, R. J. Dwayne. Miller, A. Münscher, C. Dalchow, Otology & Neurotology 39(4), pp. E224-e230 (2018). This work shows the application of PIRL for recovery of hearing loss (stapes reconstruction). This and work on sclerostomy (see Linke et al in full list of publications) illustrated important applications in both recovery of hearing and vision (treatment for glaucoma).
“Capturing Chemistry in Action with Electrons: Realization of Atomically Resolved Reaction Dynamics” by A. A. Ischenko, P. M. Weber, and R. J. Dwayne Miller, Chemical Reviews 117 (16), pp. 11066–11124 (2017). This review documents the literature for the achievement of the first atomic movies. This term is defined as a direct observation of atomic motion - with the sub-Å spatial resolution relevant to chemical processes, and sufficient time resolution to resolve the relative atomic motions faster than collisions or energy redistribution in vibrational modes blur out the spatial correlations/forces involved. This review gives the history of this achievement at the U of Toronto that has led to the formation a new conceptual basis for chemistry
“The Primary Photochemistry of Vision Occurs at the Molecular Speed Limit” by P. J. M. Johnson, M. Farag, A. Halpin, T. Morizumi, V. Prokhorenko, J. Knoester, T. L. C Jansen, O. P. Ernst, R. J. Dwayne Miller: The Journal of Physical Chemistry B (2017). Fundamental limit to chemistry found in nature. Perspective given by Rich Mathies re: Nature Chem.
“Low-dose cryo electron ptychography via non-convex Bayesian optimization” by P. Pelz, W. X. Qiu, R. Bücker, G. Kassier, and R. J. Dwayne Miller, Scientific Reports 7 (2017). This work demonstrates a reduction in electron dose by 100x which is critical to image purity (avoid damage) and is the first step towards atomically resolved single biological molecules in action.
Invited Lectures and Papers Presented
From 2008 – 2022, over 200 presentations were made with over 150 of these being invited lectures, Named Lectures, Gordon Conferences, Faraday Discussions, Max Born Institute, DESY, Riken, Kyoto, Institute for Molecular Science (Okazaki), Nagoya, Columbia, Yale, MIT, UC Boulder Distinguished Summer Lecture Series, Princeton, Stanford, Global Lecturer (Japan), Student Invited Colloquia (Chicago, Emory, Stanford) etc.
Fellow of the Royal Society, European Physical Society Prize for Laser Science, Fellow of Royal Society of Canada, Fellow of Royal Society of Chemistry, A.P. Sloan Fellowship, Camille and Henry Dreyfus Fellowship, Guggenheim Fellowship, Humboldt Award, Presidential Young Investigator, Rutherford Medal in Chemistry, CIC Medal, McNeil Medal for Science Promotion
R. J. Dwayne Miller has published over 300 research articles, one book, and several reviews. He made seminal contributions to the development of coherent multidimensional spectroscopy methods and associated ultrafast laser technology, and most notably pioneered the development of ultrabright electron sources to probe structural dynamics. The electron sources developed by his group are sufficiently bright to literally light up atomic motions in real time. He and his group were the first to capture atomic motions during the defining moments of chemistry – to directly observe the very essence of chemistry. This work accomplished one of the dream experiments in science, to bring the chemists’ collective gedankenexperiment of chemistry to direct observation. It is forming the basis for a new conceptual model for chemistry based on key reaction modes that unifies structure and dynamics to guide chemical intuition. As a testimony to the importance of basic research, the very first atomic movie provided new insight into strongly driven phase transitions involved in laser ablation that led to the ultimate limit in minimally invasive laser surgery with intact molecular signatures for guidance, and scar free healing. His research accomplishments have been recognized with an A.P. Sloan Fellowship, Camille and Henry Dreyfus Teacher-Scholar Award, Guggenheim Fellowship, Presidential Young Investigator Award (USA), Polanyi Award, Rutherford Medal in Chemistry, the Chemical Institute of Canada (CIC) Medal, Humboldt Fellowship, and numerous named lectureships. He was inducted as a Fellow of the Royal Society of Canada, Fellow of the Canadian Institute of Chemistry, Fellow of the Optical Society of America, and distinguished University Professor at the University of Toronto. He received the E. Bright Wilson Award in Spectroscopy, conferred by the American Chemical Society (2015), the Centenary Prize from the Royal Society of Chemistry (2016), and Doctorate of Science Degree (honoris causa) from the University of Waterloo (2017). He received (Sept 2018) the European Physical Award for Laser Science for “Achieving the Fundamental Limit to Min. Invasive Surgery with Complete Biodiagnostics ...” recognizing an important advance in medical applications. He is also a strong advocate for science promotion earning the McNeil Medal from the Royal Society of Canada (2011) for founding Science Rendezvous, which is the largest celebration of science with over 300 events all across Canada with new initiatives for remote communities in the North, aimed to make science accessible to the general public with over 215,000 attendees annually, made possible by >6000 volunteers/researchers. In 2023, R. J. Dwayne Miller was inducted as a Fellow of the Royal Society.