An official website of the United States government
Abstract Electron transfer is a fundamental process in chemistry, biology, and physics. One of the most intriguing questions concerns the realization of the transitions between nonadiabatic and adiabatic regimes of electron transfer. Using colloidal quantum dot molecules, we computationally demonstrate how the hybridization energy (electronic coupling) can be tuned by changing the neck dimensions and/or the quantum dot sizes. This provides a handle to tune the electron transfer from the incoherent nonadiabatic regime to the coherent adiabatic regime in a single system. We develop an atomistic model to account for several states and couplings to the lattice vibrations and utilize the mean-field mixed quantum-classical method to describe the charge transfer dynamics. Here, we show that charge transfer rates increase by several orders of magnitude as the system is driven to the coherent, adiabatic limit, even at elevated temperatures, and delineate the inter-dot and torsional acoustic modes that couple most strongly to the charge transfer dynamics.
more »
« less
Long-lived quantum coherent dynamics of a Λ-system driven by a thermal environment
We present a theoretical study of quantum coherent dynamics of a three-level Λ-system driven by a thermal environment (such as blackbody radiation), which serves as an essential building block of photosynthetic light-harvesting models and quantum heat engines. By solving nonsecular Bloch–Redfield master equations, we obtain analytical results for the ground-state population and coherence dynamics and classify the dynamical regimes of the incoherently driven Λ-system as underdamped and overdamped depending on whether the ratio Δ/[ rf( p)] is greater or less than one, where Δ is the ground-state energy splitting, r is the incoherent pumping rate, and f( p) is a function of the transition dipole alignment parameter p. In the underdamped regime, we observe long-lived coherent dynamics that lasts for τ c ≃ 1/ r, even though the initial state of the Λ-system contains no coherences in the energy basis. In the overdamped regime for p = 1, we observe the emergence of coherent quasi-steady states with the lifetime τ c = 1.34( r/Δ 2 ), which have a low von Neumann entropy compared to conventional thermal states. We propose an experimental scenario for observing noise-induced coherent dynamics in metastable He* atoms driven by x-polarized incoherent light. Our results suggest that thermal excitations can generate experimentally observable long-lived quantum coherent dynamics in the ground-state subspace of atomic and molecular Λ-systems in the absence of coherent driving.
more »
« less
- Award ID(s):
- 1912668
- PAR ID:
- 10424845
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 157
- Issue:
- 12
- ISSN:
- 0021-9606
- Page Range / eLocation ID:
- 124302
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Embedding tunable quantum emitters in a photonic bandgap structure enables control of dissipative and dispersive interactions between emitters and their photonic bath. Operation in the transmission band, outside the gap, allows for studying waveguide quantum electrodynamics in the slow-light regime. Alternatively, tuning the emitter into the bandgap results in finite-range emitter–emitter interactions via bound photonic states. Here, we couple a transmon qubit to a superconducting metamaterial with a deep sub-wavelength lattice constant (λ/60). The metamaterial is formed by periodically loading a transmission line with compact, low-loss, low-disorder lumped-element microwave resonators. Tuning the qubit frequency in the vicinity of a band-edge with a group index ofng = 450, we observe an anomalous Lamb shift of −28 MHz accompanied by a 24-fold enhancement in the qubit lifetime. In addition, we demonstrate selective enhancement and inhibition of spontaneous emission of different transmon transitions, which provide simultaneous access to short-lived radiatively damped and long-lived metastable qubit states.more » « less
-
We demonstrate efficient filtering of coherent light from a broad spectral background. A Michelson interferometer is used to effectively filter out the coherent emission of mid-infrared lasers from the co-propagating incoherent emission of a broadband thermal source. We show coherent light suppression as high as 16.9 dB without any modification of the broadband incoherent background spectrum. In addition, we demonstrate the ability to measure the spatially dependent (incoherent) thermal emission from a patterned surface, using our filter to remove a coherent signal which would otherwise overload our detection system. The demonstrated filter is rapidly tunable and wavelength-flexible, and has potential for imaging and spectroscopy applications in the presence of an otherwise overpowering coherent signal.more » « less
-
Quantum many-body scar states are highly excited eigenstates of many-body systems that exhibit atypical entanglement and correlation properties relative to typical eigenstates at the same energy density. Scar states also give rise to infinitely long-lived coherent dynamics when the system is prepared in a special initial state having finite overlap with them. Many models with exact scar states have been constructed, but the fate of scarred eigenstates and dynamics when these models are perturbed is difficult to study with classical computational techniques. In this work, we propose state preparation protocols that enable the use of quantum computers to study this question. We present protocols both for individual scar states in a particular model, as well as superpositions of them that give rise to coherent dynamics. For superpositions of scar states, we present both a system-size-linear depth unitary and a finite-depth nonunitary state preparation protocol, the latter of which uses measurement and postselection to reduce the circuit depth. For individual scarred eigenstates, we formulate an exact state preparation approach based on matrix product states that yields quasipolynomial-depth circuits, as well as a variational approach with a polynomial-depth ansatz circuit. We also provide proof of principle state-preparation demonstrations on superconducting quantum hardware.more » « less
-
Abstract In the superradiant phase transition (SRPT), coherent light and matter fields are expected to appear spontaneously in a coupled light–matter system in thermal equilibrium. However, such an equilibrium SRPT is forbidden in the case of charge-based light–matter coupling, known as no-go theorems. Here, we show that the low-temperature phase transition of ErFeO3at a critical temperature of approximately 4 K is an equilibrium SRPT achieved through coupling between Fe3+magnons and Er3+spins. By verifying the efficacy of our spin model using realistic parameters evaluated via terahertz magnetospectroscopy and magnetization experiments, we demonstrate that the cooperative, ultrastrong magnon–spin coupling causes the phase transition. In contrast to prior studies on laser-driven non-equilibrium SRPTs in atomic systems, the magnonic SRPT in ErFeO3occurs in thermal equilibrium in accordance with the originally envisioned SRPT, thereby yielding a unique ground state of a hybrid system in the ultrastrong coupling regime.more » « less
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0102808
