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arXiv:2606.04295

Quantum digital simulations of time-domain semiconductor spectroscopy in the semi-classical approximation

Mykhailo Klymenko, Bahar Goldozian, Thong Hoang, Jared H. Cole, Muhammad Usman

quant-phSubmitted Jun 2, 2026• Announced Jun 4, 2026• 0 citations• Revised Oct 25, 2026 (v2)
v1 · Jun 2, 2026v2 · Oct 25, 2026
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Abstract

We present a digital quantum simulation framework for ultrafast optical spectroscopy of semiconductor materials. The framework is based on Brillouin-zone discretization and is designed as a quantum alternative to classical simulations based on the semiconductor Bloch equations. Its current capabilities include quantum simulations of linear absorption and optical gain, incorporating Lorentzian broadening, finite-temperature band-filling effects, and reduced-dimensionality effects. Comparison with classical simulations of GaAs within the single-particle approximation demonstrates quantitative agreement in the noiseless limit. The inclusion of realistic hardware noise characteristic of NISQ-era quantum computers effectively manifests as an additional source of scattering, resulting in increased spectral broadening. We also show that the linear optical response, including many-body interactions treated within the Hartree-Fock approximation, can be mapped onto a system of coupled classical oscillators. Under certain assumptions about the query complexity of the oscillator couplings, this system exhibits a provable quantum advantage, as demonstrated in [Phys. Rev. X 13, 041041 (2023)]. Beyond the Hartree-Fock approximation, classical simulations based on many-body quantum kinetic equations face the so-called hierarchy problem, whereas the algorithmic complexity of the quantum simulations remains unchanged, offering a promising approach to overcoming this challenge.

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We present a digital quantum simulation framework for ultrafast optical spectroscopy of semiconductor materials. The framework is based on Brillouin-zone discretization and is designed as a quantum alternative to classical simulations based on the semiconductor Bloch equations. Its current capabilities include quantum simulations of linear absorption and optical gain, incorporating Lorentzian broadening, finite-temperature band-filling effects, and reduced-dimensionality effects. Comparison with classical simulations of GaAs within the single-particle approximation demonstrates quantitative agreement in the noiseless limit. The inclusion of realistic hardware noise characteristic of NISQ-era quantum computers effectively manifests as an additional source of scattering, resulting in increased spectral broadening. We also show that the linear optical response, including many-body interactions treated within the Hartree-Fock approximation, can be mapped onto a system of coupled classical oscillators. Under certain assumptions about the query complexity of the oscillator couplings, this system exhibits a provable quantum advantage, as demonstrated in [Phys. Rev. X 13, 041041 (2023)]. Beyond the Hartree-Fock approximation, classical simulations based on many-body quantum kinetic equations face the so-called hierarchy problem, whereas the algorithmic complexity of the quantum simulations remains unchanged, offering a promising approach to overcoming this challenge.
Multidimensional optical spectroscopies are powerful techniques to investigate energy transfer pathways in natural and artificial systems. Because of the high information content of the spectra, numerical simulations of the optical response are of primary importance to assist the interpretation of spectral features. However, the increasing complexity of the investigated systems and their quantum dynamics call for the development of novel simulation strategies. In this work, we consider using digital quantum computers. By combining quantum dynamical simulation and nonlinear response theory, we present a quantum algorithm for computing the optical response of molecular systems. The quantum advantage stems from the efficient quantum simulation of the dynamics governed by the molecular Hamiltonian, and it is demonstrated by explicitly considering exciton-vibrational coupling. The protocol is tested on a near-term quantum device, providing the digital quantum simulation of the linear and nonlinear response of simple molecular models.
Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system sizes unless drastic approximations are made. Quantum computer could potentially overcome these classically intractable computational tasks, but existing approaches using quantum computers to simulate spectroscopy can only handle isolated and static molecules. In this work we develop a workflow that combines multi-scale modeling and time-dependent variational quantum algorithm to compute the linear spectroscopy of systems interacting with their condensed-phase environment via the relevant time correlation function. We demonstrate the feasibility of our approach by numerically simulating the UV-Vis absorption spectra of organic semiconductors. We show that our dynamical approach captures several spectral features that are otherwise overlooked by static methods. Our method can be directly used for other linear condensed-phase spectroscopy and could potentially be extended to nonlinear multi-dimensional spectroscopy.
Spectroscopy is an indispensable tool for understanding the structures and dynamics of molecular systems. However, computational modeling of spectroscopy is challenging due to the exponential scaling of computational complexity with system sizes unless drastic approximations are made. Quantum computers could potentially overcome these classically intractable computational tasks, but the existing approaches using quantum computers to simulate spectroscopy can only handle isolated and static molecules. In this work, we develop a workflow that combines multi-scale modeling and a time-dependent variational quantum algorithm to compute the linear spectroscopy of systems interacting with their condensed-phase environment via the relevant time correlation function. We demonstrate the feasibility of our approach by numerically simulating the UV-vis absorption spectra of organic semiconductors. We show that our dynamical approach captures several spectral features that are otherwise overlooked by static methods. Our method can be directly used for other linear condensed-phase spectroscopy and could potentially be extended to nonlinear multi-dimensional spectroscopy.
Ultrafast nonlinear optical spectroscopy is used to study the coherent dynamics of optically excited electron-hole pairs in semiconductors. Coulomb interaction implies that the optical inter-band transitions are dominated, at least at low temperatures, by excitonic effects. They are further enhanced in quantum confined lower-dimensional systems, where exciton and biexciton effects dominate the spectra even at room temperature. The coherent dynamics of excitons are at modest densities well described by the optical Bloch equations and a number of the dynamical effects known from atomic and molecular systems are found and studied in the exciton-biexciton system of semiconductors. At densities where strong exciton interactions, or many-body effects, become dominant, the semiconductor Bloch equations present a more rigorous treatment of the phenomena. Ultrafast degenerate four-wave mixing is used as a tool to study the coherent exciton dynamics, and the importance of performing transform limited spectroscopy is demonstrated throughout.
Modern computational techniques used to simulate quantum chemistry are on the boundary of tractability due to the exponential growth of the molecular wavefunction, requiring a careful balance between molecule size and simulation accuracy. In recent years, quantum computing has risen in popularity as a potential alternative to conventional (classical) techniques; however, most methods rely on access to "digital" quantum computers composed of qubits and quantum gates, which at present are severely limited by noise. We have developed a real-time, analog approach to simulate vibronic chemical dynamics with existing quantum technology. Our approach uses an intuitive mapping of molecular electronic and vibrational degrees of freedom onto quantum resonators and qudit (d-level system) states, with controllable couplings between degrees of freedom. The measurement output can be mapped onto different time-dependent observables, including the time-domain simulation of vibronic spectra. Our approach can also incorporate controlled sources of noise to simulate system-bath interactions and dissipative dynamics at a minimal cost. We present experimental results using a trapped-ion device, thus showing the potential for near-term simulation of chemical dynamics in complex environments beyond the abilities of classical computers.
Quantum computation provides new avenues for the simulation of complex systems, which are beyond the capability of classical computation. In this paper, we describe an efficient simulator for quantum computing models, particularly designed for simulating complex systems. Through hybrid quantum–classical methods, noise-tolerant algorithms, and adaptive parameter updating, the method addresses several limitations of NISQ-era methods. The framework proves to be more scalable, accurate, and domain-transparent in applications to molecular dynamics, material science, and quantum chemistry. Experimental results verify the benefit compared to the state of the art in terms of both convergence rate and fidelity, demonstrating its applicability for future simulation tasks.