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  1. Alluvial fans are found across a range of climates and are built from a combination of fluvial and debris flow processes. Correct identification of process is critical to reconstructing the climate and water histories of alluvial fans on Earth and Mars. Theory and data from subaerial Earth fans are often used to estimate paleoflow discharges and sediment fluxes for martian fans; however, most terrestrial work has been conducted on fans that are in hot, dry climates with runoff sourced from rainfall. This differs from the prevailing interpretation that martian fans were sourced from snowmelt under warming periglacial conditions. To characterize processes and rates of periglacial fan formation, we conducted a field-based study of the Black Mountain alluvial fan in the Aklavik Range, Canada. We observed active fluvial bedload transport as well as several small debris flows that had initiated from ice-filled gullies. Following a runoff event of ∼0.005 mm/hr to ∼0.2 mm/hr across the fan, we estimated sediment fluxes of ∼0.04 m3/hr. Under bankfull conditions, we estimated runoff rates between ∼0.01 mm/hr to ∼14 mm/hr and corresponding sediment fluxes of ∼0.3 m3/hr to ∼550 m3/hr. This suggests that moderate flow events, well below the maximum runoff production rates suggested formore »Mars, are capable of entraining and transporting appreciable amounts of sediment by fluvial processes. However, sedimentological and geomorphological observations suggest that ∼67% of the fan was deposited fluvially; the remainder was deposited by mass flows. Our results emphasize the need to take care in interpreting martian sedimentary processes and climate from fan surface morphology alone.« less
    Free, publicly-accessible full text available July 28, 2023
  2. The concerted interplay between reactive nuclear and electronic motions in molecules actuates chemistry. Here, we demonstrate that out-of-plane torsional deformation and vibrational excitation of stretching motions in the electronic ground state modulate the charge-density distribution in a donor-bridge-acceptor molecule in solution. The vibrationally-induced change, visualised by transient absorption spectroscopy with a mid-infrared pump and a visible probe, is mechanistically resolved by ab initio molecular dynamics simulations. Mapping the potential energy landscape attributes the observed charge-coupled coherent nuclear motions to the population of the initial segment of a double-bond isomerization channel, also seen in biological molecules. Our results illustrate the pivotal role of pre-twisted molecular geometries in enhancing the transfer of vibrational energy to specific molecular modes, prior to thermal redistribution. This motivates the search for synthetic strategies towards achieving potentially new infrared-mediated chemistry.
    Free, publicly-accessible full text available August 17, 2023
  3. Abstract

    Ultrafast electron diffraction and time-resolved serial crystallography are the basis of the ongoing revolution in capturing at the atomic level of detail the structural dynamics of molecules. However, most experiments capture only the probability density of the nuclear wavepackets to determine the time-dependent molecular structures, while the full quantum state has not been accessed. Here, we introduce a framework for the preparation and ultrafast coherent diffraction from rotational wave packets of molecules, and we establish a new variant of quantum state tomography for ultrafast electron diffraction to characterize the molecular quantum states. The ability to reconstruct the density matrix, which encodes the amplitude and phase of the wavepacket, for molecules of arbitrary degrees of freedom, will enable the reconstruction of a quantum molecular movie from experimental x-ray or electron diffraction data.

  4. Photosynthesis is a highly optimized process from which valuable lessons can be learned about the operating principles in nature. Its primary steps involve energy transport operating near theoretical quantum limits in efficiency. Recently, extensive research was motivated by the hypothesis that nature used quantum coherences to direct energy transfer. This body of work, a cornerstone for the field of quantum biology, rests on the interpretation of small-amplitude oscillations in two-dimensional electronic spectra of photosynthetic complexes. This Review discusses recent work reexamining these claims and demonstrates that interexciton coherences are too short lived to have any functional significance in photosynthetic energy transfer. Instead, the observed long-lived coherences originate from impulsively excited vibrations, generally observed in femtosecond spectroscopy. These efforts, collectively, lead to a more detailed understanding of the quantum aspects of dissipation. Nature, rather than trying to avoid dissipation, exploits it via engineering of exciton-bath interaction to create efficient energy flow.
  5. The Lunar Occultation Explorer (LOX) is a paradigm shift that will leverage the power of a new observational paradigm to transform our understanding of the nuclear cosmos (0.1-10 MeV) and establish the Moon as a platform for astrophysics.