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Experimental Quantum Optical Approximation of Vibronic Spectroscopy

William R. Clements, Jelmer J. Renema, A. Eckstein, Antonio A. Valido, Adriana E. Lita, Thomas Gerrits, Sae Woo Nam, W. Steven Kolthammer, Joonsuk Huh, Ian A. Walmsley

Published Oct 24, 2017• 2 citations
OpenAlex

Abstract

Molecular vibronic spectra can be used to derive the structural properties of molecules. Although there is no known efficient classical algorithm for calculating these spectra, it has recently been shown that an ideal quantum optics simulator can in principle be used to efficiently perform this calculation. In this work, we demonstrate that imperfect quantum simulators can also yield approximations of these spectra, and illustrate our findings using a proof of principle experimental simulation of the partial vibronic spectrum of tropolone. Specifically, we demonstrate a method for designing an experiment in the presence of imperfections, show that the error on the resulting estimations of vibronic spectra can be efficiently bounded, and show that such experiments can outperform a classicality criterion. Our findings provide a roadmap for future simulations of large molecules beyond the reach of current classical computers.

Related papers

Approximating vibronic spectroscopy with imperfect quantum optics

Antonio A. Valido, William R. Clements, Jelmer J. Renema +7 more

We study the impact of experimental imperfections on a recently proposed protocol for performing quantum simulations of vibronic spectroscopy. Specifically, we propose a method for quantifying the impact of these imperfections, optimizing an experiment to account for them, and benchmarking the results against a classical simulation method. We illustrate our findings using a proof of principle experimental simulation of part of the vibronic spectrum of tropolone. Our findings will inform the design of future experiments aiming to simulate the spectra of large molecules beyond the reach of current classical computers.

•Nov 23, 2018•29 citations

Approximating vibronic spectroscopy with imperfect quantum optics

William R Clements, Jelmer J Renema, A. Eckstein +7 more

We study the impact of experimental imperfections on a recently proposed protocol for performing quantum simulations of vibronic spectroscopy. Specifically, we propose a method for quantifying the impact of these imperfections, optimizing an experiment to account for them, and benchmarking the results against a classical simulation method. We illustrate our findings using a proof of principle experimental simulation of part of the vibronic spectrum of tropolone. Our findings will inform the design of future experiments aiming to simulate the spectra of large molecules beyond the reach of current classical computers.

arXiv:1710.08655•Journal of Physics B Atomic Molecular and Optical Physics•Nov 12, 2018•39 citations

Quantum Algorithm for Calculating Molecular Vibronic Spectra

Nicolas P. D. Sawaya, Joonsuk Huh

We present a quantum algorithm for calculating the vibronic spectrum of a molecule, a useful but classically hard problem in chemistry. We show several advantages over previous quantum approaches: vibrational anharmonicity is naturally included; after measurement, some state information is preserved for further analysis; and there are potential error-related benefits. Considering four triatomic molecules, we numerically study truncation errors in the harmonic approximation. Further, in order to highlight the fact that our quantum algorithm's primary advantage over classical algorithms is in simulating anharmonic spectra, we consider the anharmonic vibronic spectrum of sulfur dioxide. In the future, our approach could aid in the design of materials with specific light-harvesting and energy transfer properties, and the general strategy is applicable to other spectral calculations in chemistry and condensed matter physics.

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Predicting molecular vibronic spectra using time-domain analog quantum simulation

Ryan J. MacDonell, Tomas Navickas, Tim F. Wohlers-Reichel +8 more

Spectroscopy is one of the most accurate probes of the molecular world. However, predicting molecular spectra accurately is computationally difficult because of the presence of entanglement between electronic and nuclear degrees of freedom. Although quantum computers promise to reduce this computational cost, existing quantum approaches rely on combining signals from individual eigenstates, an approach that is difficult to scale because the number of eigenstates grows exponentially with molecule size. Here, we introduce a method for scalable analog quantum simulation of molecular spectroscopy, by performing simulations in the time domain. Our approach can treat more complicated molecular models than previous ones, requires fewer approximations, and can be extended to open quantum systems with minimal overhead. We present a direct mapping of the underlying problem of time-domain simulation of molecular spectra to the degrees of freedom and control fields available in a trapped-ion quantum simulator. We experimentally demonstrate our algorithm on a trapped-ion device, exploiting both intrinsic electronic and motional degrees of freedom, showing excellent quantitative agreement for a single-mode vibronic photoelectron spectrum of SO$_2$.

arXiv:2209.06558•Sep 14, 2022•7 citations

MODELLING MOLECULES WITH IONS AND LASERS: ANALOG QUANTUM SIMULATION OF TIME-DOMAIN SPECTROSCOPY AND BEYOND

Ryan J. MacDonell

For roughly a century, spectroscopy has been our window into the molecular domain. It has served as a benchmark for the development of new theoretical methods in quantum chemistry, which in turn have aided the assignment and characterization of molecular spectra. The advent of quantum computing is no exception. Quantum computers have the potential to greatly increase the scale and accuracy of simulated molecular systems. However, current "digital" quantum computers will remain limited in size and number of operations in the near future due to environmental noise. Conversely, analog quantum computers may be used to simulate realistic molecular systems with current technology. They consist of controllable quantum devices with a system-specific mapping onto a quantum system of interest, such as a molecule. I will present our recent work on the development of an analog quantum toolkit for the simulation of vibronic coupling Hamiltonians, including the prediction of vibronic spectra. I will show the theoretical capabilities and limits of our approach, and show proof-of-principle experimental results from collaborators. Finally, I will discuss what is next in the exciting world of analog quantum simulation.

International Symposium on Molecular Spectroscopy (ISMS)•Jun 22, 2023•0 citations

Linear quantum optics: components and applications

William R. Clements

Quantum optics has successfully been used to test fundamental principles in quantum physics and to demonstrate the potential of quantum-enhanced technologies. Linear quantum optics, in which large quantum states of light are produced by optical interference of smaller quantum states, has proved to be particularly fruitful. Further progress will rely both on developing improved experimental tools to manipulate and measure quantum light, and on expanding and refining the range of applications of these technologies. This thesis presents our contributions towards both of these endeavours. We first focus on some of the components necessary for linear quantum optics, starting with the requirement for reconfigurable interference between several optical modes. We propose a novel design for interferometers that satisfy this requirement, which is based on a new mathematical decomposition of unitary matrices used to describe optical interference. We show that our design is more efficient than previously known designs. We also experimentally demonstrate a modular approach to building these devices, which is based on the assembly of multiple UV-written integrated photonic chips. These chips are characterised, and three of them are assembled into a structure shown to enable a wide range of optical transformations. We then study methods of photon detection, showing how photon detectors can be calibrated and discussing the operation of superconducting photon number resolving transition edge sensors. Next, we study two applications of linear optics. We examine the applicability of a proposal for simulating molecular spectroscopy using quantum optics in the presence of experimental imperfections. Our findings are illustrated with a proof of principle experiment in which we simulate part of the vibronic spectrum of the tropolone molecule. Finally, we study a class of optical devices, known as optical Ising machines, that has been shown to find solutions to difficult combinatorial problems. Describing the optical pulses in these devices in phase space as Gaussian quasi-probability distributions that evolve stochastically, we analyse the computational mechanism of these machines and show in theory that they can be simplified without affecting their performance.

•Jan 1, 2018•3 citations
Molecular vibronic spectra can be used to derive the structural properties of molecules. Although there is no known efficient classical algorithm for calculating these spectra, it has recently been shown that an ideal quantum optics simulator can in principle be used to efficiently perform this calculation. In this work, we demonstrate that imperfect quantum simulators can also yield approximations of these spectra, and illustrate our findings using a proof of principle experimental simulation of the partial vibronic spectrum of tropolone. Specifically, we demonstrate a method for designing an experiment in the presence of imperfections, show that the error on the resulting estimations of vibronic spectra can be efficiently bounded, and show that such experiments can outperform a classicality criterion. Our findings provide a roadmap for future simulations of large molecules beyond the reach of current classical computers.
We study the impact of experimental imperfections on a recently proposed protocol for performing quantum simulations of vibronic spectroscopy. Specifically, we propose a method for quantifying the impact of these imperfections, optimizing an experiment to account for them, and benchmarking the results against a classical simulation method. We illustrate our findings using a proof of principle experimental simulation of part of the vibronic spectrum of tropolone. Our findings will inform the design of future experiments aiming to simulate the spectra of large molecules beyond the reach of current classical computers.
We study the impact of experimental imperfections on a recently proposed protocol for performing quantum simulations of vibronic spectroscopy. Specifically, we propose a method for quantifying the impact of these imperfections, optimizing an experiment to account for them, and benchmarking the results against a classical simulation method. We illustrate our findings using a proof of principle experimental simulation of part of the vibronic spectrum of tropolone. Our findings will inform the design of future experiments aiming to simulate the spectra of large molecules beyond the reach of current classical computers.
We present a quantum algorithm for calculating the vibronic spectrum of a molecule, a useful but classically hard problem in chemistry. We show several advantages over previous quantum approaches: vibrational anharmonicity is naturally included; after measurement, some state information is preserved for further analysis; and there are potential error-related benefits. Considering four triatomic molecules, we numerically study truncation errors in the harmonic approximation. Further, in order to highlight the fact that our quantum algorithm's primary advantage over classical algorithms is in simulating anharmonic spectra, we consider the anharmonic vibronic spectrum of sulfur dioxide. In the future, our approach could aid in the design of materials with specific light-harvesting and energy transfer properties, and the general strategy is applicable to other spectral calculations in chemistry and condensed matter physics.
Spectroscopy is one of the most accurate probes of the molecular world. However, predicting molecular spectra accurately is computationally difficult because of the presence of entanglement between electronic and nuclear degrees of freedom. Although quantum computers promise to reduce this computational cost, existing quantum approaches rely on combining signals from individual eigenstates, an approach that is difficult to scale because the number of eigenstates grows exponentially with molecule size. Here, we introduce a method for scalable analog quantum simulation of molecular spectroscopy, by performing simulations in the time domain. Our approach can treat more complicated molecular models than previous ones, requires fewer approximations, and can be extended to open quantum systems with minimal overhead. We present a direct mapping of the underlying problem of time-domain simulation of molecular spectra to the degrees of freedom and control fields available in a trapped-ion quantum simulator. We experimentally demonstrate our algorithm on a trapped-ion device, exploiting both intrinsic electronic and motional degrees of freedom, showing excellent quantitative agreement for a single-mode vibronic photoelectron spectrum of SO2_22​.
For roughly a century, spectroscopy has been our window into the molecular domain. It has served as a benchmark for the development of new theoretical methods in quantum chemistry, which in turn have aided the assignment and characterization of molecular spectra. The advent of quantum computing is no exception. Quantum computers have the potential to greatly increase the scale and accuracy of simulated molecular systems. However, current "digital" quantum computers will remain limited in size and number of operations in the near future due to environmental noise. Conversely, analog quantum computers may be used to simulate realistic molecular systems with current technology. They consist of controllable quantum devices with a system-specific mapping onto a quantum system of interest, such as a molecule. I will present our recent work on the development of an analog quantum toolkit for the simulation of vibronic coupling Hamiltonians, including the prediction of vibronic spectra. I will show the theoretical capabilities and limits of our approach, and show proof-of-principle experimental results from collaborators. Finally, I will discuss what is next in the exciting world of analog quantum simulation.
Quantum optics has successfully been used to test fundamental principles in quantum physics and to demonstrate the potential of quantum-enhanced technologies. Linear quantum optics, in which large quantum states of light are produced by optical interference of smaller quantum states, has proved to be particularly fruitful. Further progress will rely both on developing improved experimental tools to manipulate and measure quantum light, and on expanding and refining the range of applications of these technologies. This thesis presents our contributions towards both of these endeavours. We first focus on some of the components necessary for linear quantum optics, starting with the requirement for reconfigurable interference between several optical modes. We propose a novel design for interferometers that satisfy this requirement, which is based on a new mathematical decomposition of unitary matrices used to describe optical interference. We show that our design is more efficient than previously known designs. We also experimentally demonstrate a modular approach to building these devices, which is based on the assembly of multiple UV-written integrated photonic chips. These chips are characterised, and three of them are assembled into a structure shown to enable a wide range of optical transformations. We then study methods of photon detection, showing how photon detectors can be calibrated and discussing the operation of superconducting photon number resolving transition edge sensors. Next, we study two applications of linear optics. We examine the applicability of a proposal for simulating molecular spectroscopy using quantum optics in the presence of experimental imperfections. Our findings are illustrated with a proof of principle experiment in which we simulate part of the vibronic spectrum of the tropolone molecule. Finally, we study a class of optical devices, known as optical Ising machines, that has been shown to find solutions to difficult combinatorial problems. Describing the optical pulses in these devices in phase space as Gaussian quasi-probability distributions that evolve stochastically, we analyse the computational mechanism of these machines and show in theory that they can be simplified without affecting their performance.