arXiv:2411.16290 · Physical Review Research

Accelerating two-dimensional electronic spectroscopy simulations with a probe qubit protocol

José D. Guimarães, James Lim, Mikhail I. Vasilevskiy, Susana F. Huelga, Martin Bodo Plenio

Published May 9, 2025• 5 citations

Abstract

Two-dimensional electronic spectroscopy (2DES) is a powerful tool for exploring quantum effects in energy transport within photosynthetic systems and investigating novel material properties. However, simulating the dynamics of these experiments poses significant challenges for classical computers due to the large system sizes, long timescales, and numerous experiment repetitions involved. This paper introduces the probe qubit protocol (PQP)-for quantum simulation of 2DES on quantum devices-addressing these challenges. The PQP offers several enhancements over standard methods, notably reducing computational resources, by requiring only a single-qubit measurement per circuit run and achieving Heisenberg scaling in detection frequency resolution, without the need to apply expensive controlled evolution operators in the quantum circuit. The implementation of the PQP protocol requires only one additional ancilla qubit, the probe qubit, with one-to-all connectivity and two-qubit interactions between each system and probe qubits. We evaluate the computational resources necessary for this protocol in detail, demonstrating its function as a dynamic frequency-filtering method through numerical simulations. We find that simulations of the PQP on classical and quantum computers enable a reduction on the number of measurements, i.e., simulation runtime, and memory savings of several orders of magnitude relative to standard quantum simulation protocols of 2DES. The paper discusses the applicability of the PQP on near-term quantum devices and highlights potential applications where this spectroscopy simulation protocol could provide significant speedups over standard approaches such as the quantum simulation of 2DES applied to the Fenna-Matthews-Olson (FMO) complex in green sulfur bacteria.

DOI: 10.1103/physrevresearch.7.023130

Related papers

Quantum simulator of an open quantum system using superconducting qubits: exciton transport in photosynthetic complexes

Sarah Mostame, Patrick Rebentrost, Alexander Eisfeld +3 more

Open quantum system approaches are widely used in the description of physical, chemical and biological systems. A famous example is electronic excitation transfer in the initial stage of photosynthesis, where harvested energy is transferred with remarkably high efficiency to a reaction center. This transport is affected by the motion of a structured vibrational environment, which makes simulations on a classical computer very demanding. Here we propose an analog quantum simulator of complex open system dynamics with a precisely engineered quantum environment. Our setup is based on superconducting circuits, a well established technology. As an example, we demonstrate that it is feasible to simulate exciton transport in the Fenna–Matthews–Olson photosynthetic complex. Our approach allows for a controllable single-molecule simulation and the investigation of energy transfer pathways as well as non-Markovian noise-correlation effects.

arXiv:1106.1683New Journal of PhysicsOct 10, 2012104 citations

How can the green sulfur bacteria use quantum computing for light harvesting?

D. Drakova, G. Doyen

Long lasting coherence in photosynthetic pigment-protein complexes has been observed even at physiological temperatures. Experiments have demonstrated quantum coherent behaviour in the long-time operation of the D-Wave quantum computer as well. Quantum coherence is the common feature between the two phenomena. An explanations for eight orders of magnitude discrepancy between the single flux qubit coherence time and the long-time quantum behaviour of an array of thousand flux qubits in the quantum computer was suggested within a theory where the flux qubits are coupled to an environment of particles called gravonons of high density of states The coherent evolution is in high dimensional spacetime and can be understood as a solution of Schroedinger's time-dependent equation. Explanations for the quantum beats observed in 2D Fourier transform electronic spectroscopy of the Fenna-Matthews-Olson (FMO) protein complex in the green sulfur bacteria are presently sought in constructing transport theories based on quantum master equations where 'good' molecular vibrations ('coloured noise') in the chlorophyll and the surrounding protein scaffold knock the exciton oscillations back into coherence. These 'good' vibrations are claimed to have developed in three billion years of natural selection. These theories, however, face the discomforting experimental observation that "attempts to scramble vibrational modes or to shift resonances with isotopic substitution miserably failed to affect the beating signals". As a possible way out of this dilemma we adopted the formalism of the quantum computation to the quantum beats in the FMO protein complex.

arXiv:1605.06149May 11, 20162 citations

Characterising many-body systems via quantum dynamics simulations

Lucia Vilchez-Estevez

Simulating quantum many-body systems is essential for understanding complex phenomena in condensed matter, chemistry, and materials science. Quantum computing offers a way to overcome the limitations of classical methods by operating directly in exponentially large Hilbert spaces. In particular, classical methods often fail to capture the dynamics of strongly correlated systems, which makes quantum algorithms a promising alternative for exploring these challenging regimes. This thesis uses quantum dynamics simulations to probe the behaviour of many-body systems. We first introduce a spectroscopy-based protocol to extract excitation spectra from the time evolution of observables and analyse its performance on near-term quantum devices. We show that the protocol requires only short evolution times and is resilient to errors, facilitating its implementation on real hardware. Building on this, we simulate fermionic excitation spectra using current quantum devices, introducing resource optimisations - including an approximate free-fermion initial state, a unitary quench without ancillae, and reduced Trotter steps - that significantly lower circuit depth. These improvements enable simulations at system sizes competitive with the state of the art, yielding results that match classical benchmarks. While most studies focus on unitary dynamics of isolated systems, open quantum dynamics is increasingly relevant for describing non-equilibrium processes across biology, materials science, and quantum control. We extend our scope to systems coupled to an environment and governed by Lindbladian evolution. By studying simulation complexity through physically meaningful quantities - such as correlation length and mixing time - we explore whether open-system dynamics can be as tractable as their unitary counterparts. These findings provide insights into the computational complexity landscape of open-system simulation and highlight regimes where quantum methods offer a clear advantage.

Jan 1, 20250 citations

Understanding and manipulating electronic quantum coherence in photosynthetic light-harvesting

Stephan Hoyer

Ultrafast spectroscopy experiments show that photosynthetic systems can preserve quantum beats in the process of electronic energy transfer between pigments, even at room temperature. But what does this discovery imply for biology - and for quantum mechanics? This dissertation examines photosynthesis through the tools of quantum information science. We evaluate to what extent photosynthesis can be thought of as a type of quantum technology, and consider how we can apply experimental tools widely used for quantum technologies (state tomography and coherent control) to photosynthesis. Throughout, we use the Fenna-Matthews-Olson (FMO) complex of greens sulfur bacteria as a model photosynthetic pigment-protein complex.In Part I, we evaluate two mechanisms for the possible biological relevance of quantum coherent motion. First, we consider the extent to which dynamics in light-harvesting systems exhibit the quantum speedups characteristic of quantum algorithms and quantum walks. Second, we demonstrate a ratchet effect in electronic energy transfer enabled by partially coherent dynamics. To do so, we build a new model of energy transfer between weakly coupled light-harvesting complexes to understand how electronic coherence arises under natural conditions.In Part II, we present proposals for experimental probes of light harvesting dynamics with ultrafast spectroscopy. We show how the signal from pump-probe spectroscopy can be formally inverted to determine the excited state electronic density matrix. Finally, we examine the feasiblity of coherent control experiments on light-harvesting systems, and provide two realistic targets feasible with present-day technology.

Jan 1, 20130 citations

Simulating molecules on a cloud-based 5-qubit IBM-Q universal quantum computer

Sebastian Leontica, Felix Tennie, Tristan Farrow

Abstract Simulating the behaviour of complex quantum systems is impossible on classical supercomputers due to the exponential scaling of the number of quantum states with the number of particles in the simulated system. Quantum computers aim to break through this limit by using one quantum system to simulate another quantum system. Although in their infancy, they are a promising tool for applied fields seeking to simulate quantum interactions in complex atomic and molecular structures. Here, we show an efficient technique for transpiling the unitary evolution of quantum systems into the language of universal quantum computation using the IBM quantum computer and show that it is a viable tool for compiling near-term quantum simulation algorithms. We develop code that decomposes arbitrary 3-qubit gates and implement it in a quantum simulation first for a linear ordered chain to highlight the generality of the approach, and second, for a complex molecule. We choose the Fenna-Matthews-Olsen (FMO) photosynthetic protein because it has a well characterised Hamiltonian and presents a complex dissipative system coupled to a noisy environment that helps to improve the efficiency of energy transport. The method can be implemented in a broad range of molecular and other simulation settings.

Communications PhysicsJun 2, 202123 citations

An enhanced algorithm for simulating non-unitary dynamics on quantum computers

Mader, Simon

This thesis introduces an algorithm for efficiently simulating the non-unitary dynamics of open quantum systems on quantum computers. Open quantum systems interact with their surrounding environment, resulting in non-unitary dynamics. This creates a fundamental challenge for quantum simulation, since quantum hardware is inherently restricted to unitary operations. Building on the Kraus operator sum representation, this work explores dilation techniques that embed non-unitary maps into larger unitary operations, suitable for implementation on quantum processors. In addition to reproducing recent results from the literature, an enhanced algorithm that reuses the quantum state from the previous time step is presented. This reuse strategy increases efficiency, permits repeated application of the same quantum circuit, and shifts the dominant computational workload toward the quantum processor. The method is implemented and tested on models of the Fenna–Matthews–Olson light-harvesting complex and compares the obtained results against existing approaches. Importantly, the algorithm is broadly applicable to a wide class of open quantum systems. The proposed scheme provides a practical pathway for studying transport, dynamics, and spectral properties of interacting quantum systems on a quantum simulator, while keeping the demands on classical resources modest. The thesis concludes with a discussion of implementation details, numerical results, and prospects for scaling the method to larger systems.

Jan 1, 20250 citations