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| name: Blake Simpkins | ||
| first_name: Blake | ||
| last_name: Simpkins | ||
| asociation: US Naval Research Laboratory | ||
| --- |
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| name: Luis Marcassa | ||
| first_name: Luis Gustavo | ||
| last_name: Marcassa | ||
| asociation: Instituto de Física de São Carlos, Universidade de São Paulo | ||
| --- |
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| name: Katy Aruachan | ||
| first_name: Katy | ||
| last_name: Aruachan | ||
| asociation: Universidad de Santiago de Chile | ||
| --- |
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| name: Tomasz Antosiewicz | ||
| first_name: Tomasz J. | ||
| last_name: Antosiewicz | ||
| asociation: University of Warsaw | ||
| --- |
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| name: New frontiers in quantum simulation with dipolar gases | ||
| speakers: | ||
| - Ana Maria Rey | ||
| categories: | ||
| - Talk | ||
| --- | ||
| Recent experimental developments on cooling, trapping, and manipulating ultra-cold dipolar gases are opening a door for the controllable study of their complex many-body quantum dynamics. In particular, by encoding a spin degree of freedom in rotational levels in polar molecules it is now possible to use these systems to emulate a variety of rich spin models exhibiting long range and anisotropic interactions. In this talk, I will discuss theoretical and experimental progress towards engineering quantum spin models in large molecule arrays trapped in 3D optical lattices relevant for quantum simulations and sensing. |
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| name: Suppressed reactivity via cavity-induced selective vibrational cooling | ||
| name: Materials Design through Quantum Mechanical Coupling | ||
| speakers: | ||
| - Blake Simpkins | ||
| categories: | ||
| - Talk | ||
| --- | ||
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| B. S. Simpkins, (1) W. Ahn, (2) J. F. Triana, (3) F. Recabal, (3) A. D. Dunkelberger, (1) J. C. Owrutsky, (1) F. Herrera (3,4) | ||
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| (1) Chemistry Division, U.S. Naval Research Laboratory, Washington, DC 20375, United States | ||
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| (2) UNAM National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology, Bilkent University, Ankara, Turkey | ||
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| (3) Department of Physics, Universidad de Santiago de Chile, Santiago, Chile | ||
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| (4) Millennium Institute for Research in Optics (MIRO), Chile | ||
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| Molecular vibrations can couple to optical cavities to create new hybrid states called polaritons. The magnitude of this coupling, measured as the vacuum Rabi splitting (Ω), correlates with modified materials processes such as photon emission, molecular energy transfer, and chemical reaction rates. In this talk, I will first discuss modeling and active control of cavity coupling to molecular vibrations. Next, I will discuss results indicating modified chemical reaction rates for an alcoholysis addition reaction forming urethane monomers. Cavity tuning was used to selectively couple to reactant, solvent, and product vibrational modes resulting in a chemical response that is cavity tuning dependent. An open quantum system model attempting to rationalize such reaction suppression is presented which identifies bond-selective cooling via cavity-induced stationary population redistribution as the culprit. | ||
| Sensing processes are simply a material’s response to some s1mulus. There are many conven1onal ways to tailor a material’s transduc1on response including nanostructuring to enhance surface effects, chemical func1onaliza1on for specificity, op1cal mode engineering to enhance op1cal cross-sec1on and/or tune frequency response, or system design to incorporate mul1-func1onality. In this program, we are interested in basic research aimed at dras1c or fundamental altera1ons of a material’s response to s1muli. For instance, introducing quantum mechanical coupling (interac1on) in material design is expected to improve material transduc1on and related sensing func1onality through increased sensi1vity and improved power efficiency. U1liza1on of quantum-mechanical interac1ons as a mode of materials design can take various forms. Coupling of material excita1ons (e.g., excitons, phonons, vibra1ons) to op1cal cavity modes has yielded exciton control, polariton forma1on and condensa1on, and opto-mechanical sensors opera1ng in the quantum squeezed regime. Tailored design of molecular excitonic and spin transi1ons has advanced the interroga1on of protein structure and func1on, and the examina1on of molecular-cavity optomechanical systems allows one to drive nonlinear popula1on of vibra1onal excita1ons, manipulate molecular dephasing, and influence chemical behavior. |
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| name: Quantum effects in controlled molecular dynamics | ||
| speakers: | ||
| - Christiane Koch | ||
| categories: | ||
| - Talk | ||
| --- | ||
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| Molecular quantum science and technology hinge on the exploitation of quantum eLects. In my talk I will present two such examples. (i) Quantum resonances in low-energy collisions are a sensitive probe of the intermolecular forces. Even for strong and highly anisotropic interactions, they may dominate the final quantum state distribution, as recently observed after Penning ionization of H2 molecules [1]. Theoretical predictions for the cross sections from full quantum scattering calculations involve only the approximations made when constructing the potential energy surface (PES). Changes in the shape of the PES thus translate directly into modifications of the cross sections. This can be used to to improve calculated PES, starting from the experimental data [2]. Conversely, one can also ask by how much the experimental resolution of measured cross sections must improve in order to unambiguously discriminate predictions derived from diLerent levels of ab initio electronic structure theory [3]. (ii) Moving from low energy to short time scales, I will discuss the quantum control of photoelectron circular dichroism (PECD) in the photoionization of chiral molecules. Here, the control arises from the interference of various two-photon photoionization pathways that can be manipulated by suitably shaped ionization pulses [4,5]. PECD, remarkably, requires light-matter interaction only in the electric dipole approximation even for randomly oriented molecules. This results not only in a very large dichroic eLect, but provides also a recipe for how to induce and subsequently probe chiral dynamics in initially achiral molecules [6]. The preparation of chiral superposition states with a preferred handedness may be useful in future experiments, e.g. on measuring parity violation with chiral molecules. | ||
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| [1] Margulis et al., Science 380, 77 (2023). | ||
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| [2] Horn et al., vol. 10, Science Advances 10, eadi6462 (2024). [3] Horn et al., arXiv:2408.13197. | ||
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| [4] Goetz et al., Physical Review Letters 122, 013204 (2019). [5] Goetz et al., arXiv:2104.07522. | ||
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| [6] Tikhonov et al., Science Advances 8, eade0311 (2022). |
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| name: Circuit QED with Molecular Spin Qudits | ||
| speakers: | ||
| - Fernando Luis | ||
| categories: | ||
| - Talk | ||
| --- | ||
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| Scaling up quantum processors remains very challenging, even for today’s most successful platforms. Molecular complexes, able to encode d-dimensional qudits in their electronic and nuclear spin states, can act as universal quantum processors or even correct errors [1]. I’ll discuss recent experiments aimed at exploiting these systems by coupling them to superconducting resonators [2,3]. A high cooperativity coupling to electronic and even nuclear spins has been achieved [3,4]. We also find that it is possible to couple excitations of remote, and distinct, spin ensembles by means of interactions mediated by the circuit. The results provide the basis for the control, readout and communication of spin qubits and qudits and for implementations of quantum | ||
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| [1] G. Aromí, D. Aguilà, P. Gamez, F. Luis, and O. Roubeau, Chem. Soc. Rev., 2012, 41, 537; A. Gaita-Ariño, F. Luis, S. Hill, and E. Coronado, Nature Chem., 2019, 11, 301; S. Carretta, D. Zueco, A. Chiesa, Á. Gómez-León, and F. Luis, Appl. Phys. Lett., 2021, 118, 240501; A Chiesa, P Santini, E Garlatti, F Luis, S Carretta, Reports Prog. Phys. 87, 034501 (2024). | ||
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| [2] A. Chiesa, S. Roca, S. Chicco, M.C. de Ory, A. Gómez-León, A. Gomez, D. Zueco, F. Luis, and S. Carretta, Phys. Rev. Applied, 2023, 19, 064060. | ||
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| [3] M. Rubín-Osanz, et al, Low Temp. Phys., 2024, 50, 520. | ||
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| [4] V. Rollano et al, Commun. Phys., 2022, 5, 246. |
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| --- | ||
| name: Mapping Decoherence Pathways in Molecules | ||
| speakers: | ||
| - Ignacio Franco | ||
| categories: | ||
| - Talk | ||
| --- | ||
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| To unlock the sophistication of chemistry in building complex molecular architectures to develop next-generation quantum technologies, there is a critical need to identify robust molecular design principles that can be used to generate quantum subspaces with coherences that are protected or thatarecontrollablebychemicalmeans[1]. | ||
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| Systematic progress in this direction requires not only developing experimental and theoretical methods to quantify and manipulate quantum coherences, but also an understanding of how the decoherence (or quantum noise) introduced by the environment influences the dynamics of the system and how this influence can be modulated via chemical design. In this talk, I will summarize progress in our group developing strategies to address this problem and map decoherence pathways in molecules [2-4]. These maps quantify the contributions of specific vibrations or solvent modes to the overall dephasing and dissipation of molecular-based quantum subsystems, providing means to establish the basic chemical principles of quantum decoherence phenomena. | ||
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| [1] G. D. Scholes, A. Olaya-Castro, S. Mukamel, A. Kirrander and K.K. Ni https://arxiv.org/abs/2409.04264(2024) | ||
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| [2] I. Gustin, C.W. Kim, D.W. McCamant, and I. Franco, Proc. Natl. Acad. Sci. U.S.A. 120, e2309987120 (2023) | ||
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| [3] C. W. Kim and I. Franco, J. Chem. Phys. 160, 214111 (2024) | ||
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| [4] C. W. Kim and I. Franco, J. Chem. Phys. 160, 214112 (2024) |
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| name: The short life and times of vibrational polaritons | ||
| speakers: | ||
| - Jeff Owrutsky | ||
| categories: | ||
| - Talk | ||
| --- | ||
| There is a lot of interest in vibrational polaritons because they appear to modify chemistry.1 Following the initial studies of infrared spectra of strong coupling to polymer carbonyls and metal carbonyls dissolved in solution,2,3,4 the first transient infrared absorption studies were reported for W(CO)6 in hexane which were aimed at identifying modified vibrational dynamics,5 especially for vibrationally excited polaritons, that might account for cavity modified reactions. However, clear evidence of modified vibrational dynamics for polaritons, or even convincing demonstrations of clear spectral signatures of vibrational polaritons, remains elusive. Although aspects of the signal were initially attributed to excited state polaritons, the observed transient response is dominated by polariton contraction and enhanced excited state absorption, all phenomena described by linear optical response of the bare molecules. Two dimensional infrared (2D IR) of vibration polaritons from strong coupling to W(CO)6 showed that exciting reservoir, non-polariton states can create a response that includes polariton contraction and enhanced excited state absorption.6 Analysis of 2DIR measurements of nitroprusside anion in methanol involved subtracting the reservoir, non- polariton contributions to the signal and indicted that some of the remaining response is from excited polaritons.7 This analysis was challenged by the Kubarych group who provided insight that some early time response could be due to inhomogeneities in the molecular absorption band.8,9 In order to explain this early time response, a microscopic theory that expanded on a transfer matrix model by including excitation of the reservoir band was developed for the spectroscopy of cavity- coupled molecules that includes band inhomogeneity and can predict 2DIR spectra from molecular polaritons. The theory provides a unified picture for a global understanding of recent spectroscopic experiments on molecular polaritons. There is still the question of whether vibrationally excited polaritons exist and if so, how to reveal them. | ||
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| [1] Hutchison et al., Angew. Chem., Int. Ed. 51, 1592 (2012). | ||
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| [2] Long and Simpkins, ACS Photonics 2, 130, 2015. | ||
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| [3] Shalabney et al., Nat. Comm. 6, 5981 (2015). | ||
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| [4] Long et al. et al., ACS Photonics 2, 1460 (2015). | ||
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| [5] Dunkelberger et al., Nat. Comm. 7, 13504 (2016). | ||
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| [6] Xiang et al., PNAS 201722063 (2017). | ||
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| [7] Grafton et al., Nature Comm. 12, 214 (2021). | ||
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| [8] Simpkins et al., J. Phys. Chem. Lett. 14, 983 (2023). | ||
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| [9] Duan et al., J. Phys. Chem. Lett. 12, 11406 (2021). |
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