arXiv subjects

Ivan Kassal

Publications and source records attributed to Ivan Kassal.

At least 19 recordsLinked to original sources

arXiv2026

Noise Reduction for Universal Hybrid Oscillator-Qubit Quantum Computation

Hybrid continuous-variable--discrete-variable (CV--DV) architectures process quantum information in bosonic modes and qubits, but noise limits their performance. To reduce the noise, existing DV error correction must be complemented by CV noise reduction. Existing CV noise-reduction schemes -- such as GKP-stabilizer codes -- can reduce CV noise, but only for Gaussian gates. Therefore, no current noise-reduction scheme can correct arbitrary CV--DV gates, including non-Gaussian ones. Here, we develop noise reduction for a universal CV--DV gate set, making it applicable to arbitrary CV--DV gates. We do so by introducing an ancilla qubit into a GKP-stabilizer code, allowing us to reduce the standard deviation of Gaussian displacement noise from $\sigma$ to $\tilde O(\sigma^2)$. To demonstrate the scheme, we show that it significantly reduces noise and improves fidelity in the preparation of non-Gaussian cat and Fock states.

quant-ph↗

arXiv2026

End-to-End Simulation of Chemical Dynamics on a Quantum Computer

Simulations of chemical dynamics are a powerful means for understanding chemistry. However, classical computers struggle to simulate many chemical processes, especially non-adiabatic ones, where the Born-Oppenheimer approximation breaks down. Quantum computers could simulate quantum-chemical dynamics more efficiently than classical computers, but there is currently no complete quantum algorithm for calculating dynamical observables to within a known error. Here, we develop an efficient, end-to-end quantum algorithm for simulating chemical dynamics that avoids all uncontrolled approximations (including the Born-Oppenheimer approximation) and whose error is bounded subject to mild assumptions. To do so, we treat the nuclei and the electrons on an equal footing and simulate the full molecular wavefunction on a momentum-space grid in first quantization, including all algorithmic steps: initial-state preparation, time evolution using qubitization, and measurement of chemical observables such as reaction yields and rates. Our work gives the first algorithm for quantum simulation of chemistry whose end-to-end complexity achieves sublinear scaling in the size of the grid. We achieve this by developing an exponentially faster method for initial-state-preparation. Photochemistry is a likely early application of our algorithm and we estimate resources required for end-to-end simulations of non-adiabatic dynamics of atmospherically important molecules. Classically intractable photochemical computations could be performed using resources comparable to those required for other chemical applications of quantum computing.

quant-ph↗

arXiv2026

Programmable quantum simulation of anharmonic dynamics

Continuous-variable-discrete-variable (CV-DV) quantum simulators offer a natural route to simulating bosonic dynamics relevant to many branches of physics and chemistry. However, programmable simulation of arbitrary dynamics is an outstanding challenge. In particular, simulating anharmonic dynamics, which is ubiquitous across the physical sciences, is challenging due to the highly harmonic nature of oscillators used in CV-DV simulators. Here, we experimentally demonstrate programmable CV-DV quantum simulation of anharmonic dynamics in a range of double-well potentials, implemented in a trapped-ion system. We synthesise the time-evolution operators using a bosonic-quantum-signal-processing subroutine, which allows the potential to be tuned between experiments by controlling classical experimental parameters. We observe coherent dynamics in various double-well potentials, where a wavepacket tunnels through the potential barrier, and we suppress this effect by programmatically introducing asymmetry.

quant-ph↗

arXiv2026

Delocalisation explains efficient transport and charge generation in neat Y6 organic photovoltaics

Non-fullerene acceptors (NFA), such as Y6, have significantly improved the efficiency of organic photovoltaic devices (OPVs). However, the fundamental processes behind the high efficiencies of NFA devices have remained incompletely understood, with the high efficiencies persisting without the large energetic offsets often thought to be required for charge separation. Even more surprising has been the efficient charge generation in neat Y6 devices, where there is no energetic offset at all. Here, we simulate charge transport and separation in Y6 using delocalised kinetic Monte Carlo (dKMC) parameterised using atomistic calculations, thus taking into account the often-neglected ingredients of delocalisation, disorder, and polaron formation. Including delocalisation predicts higher carrier mobilities and exciton diffusion coefficients than is possible with classical simulations, bringing them into agreement with experimental values. Delocalisation also predicts higher charge-generation efficiencies in neat Y6, in agreement with experimental measurements. Finally, this work establishes dKMC as a realistic, predictive tool for understanding next-generation OPVs.

cond-mat.mtrl-sci↗

arXiv2025

Using bosons to improve resource efficiency of quantum simulation of vibronic molecular dynamics

Simulating chemical dynamics is computationally challenging, especially for nonadiabatic dynamics, where numerically exact classical simulations scale exponentially with system size, becoming intractable for even small molecules. On quantum computers, chemical dynamics can be simulated efficiently using either universal, qubit-only devices or specialized mixed-qudit-boson (MQB) simulators, which natively host electronic and vibrational degrees of freedom. Here, we compare the quantum resources required for a qubit-only approach to achieve the same accuracy as an MQB device at simulating nonadiabatic molecular dynamics. We find that MQB simulations require orders-of-magnitude fewer quantum operations than qubit-only simulations, with a one-gate MQB circuit requiring a qubit-equivalent circuit volume of over 400,000 when simulating an isolated molecule, which increases to over ten million when environmental effects are included. These estimates assume perfect qubits and gates, and would increase by additional orders of magnitude if error correction were used for fault tolerance. When errors are small, the advantage of MQB simulators becomes even larger as system size increases. Our results highlight the enormous resource advantages of representing non-qubit chemical degrees of freedom natively, rather than encoding them into qubits.

quant-ph↗

arXiv2025

Programmable generation of arbitrary continuous-variable anharmonicities and nonlinear couplings

Harmonic oscillators are promising continuous-variable (CV) quantum resources because their infinite-dimensional Hilbert spaces allow for resource-efficient quantum computing and simulation. To reach their full potential, CV platforms need to be able to efficiently implement non-Gaussian operations. Bosonic quantum-signal-processing schemes have emerged as attractive methods to construct arbitrary non-Gaussian operations; however, these schemes are restricted to single modes, i.e., the implementation of anharmonic potentials. Here, we introduce trigonometric-gate-implemented Fourier synthesis (TGIFS), a method for implementing arbitrary non-Gaussian operations applicable to both single- and multi-mode systems, allowing the generation of both anharmonicities and nonlinear multi-mode couplings. TGIFS synthesizes a target Hamiltonian by decomposing it into a Fourier series whose terms are implemented via bosonic quantum signal processing, which uses a discrete-variable (DV) system to induce a nonlinearity in the CV system. Our hybrid CV-DV protocol allows for the direct simulation of a broad range of CV phenomena (such as those in lattice gauge theory, chemical dynamics, and quantum chaos) and provides a richer toolbox for CV circuit compilation.

quant-ph↗

arXiv2025

Unifying Collective Effects in Emission, Absorption, and Transfer

Collective effects, such as superradiance and subradiance are central to emerging quantum technologies -- from sensing to energy storage -- and play an important role in light-harvesting. These effects enhance or suppress rates of dynamic processes (absorption, emission, and transfer) due to the formation of symmetric or antisymmetric collective states. However, collective effects in different contexts -- absorption, emission, and transfer -- have often been defined disparately, especially across different communities, leading to results that are not immediately transferable between different contexts. Here, we describe all three types of collective effects using a common Dicke framework that resolves the apparent discrepancies between different approaches. It allows us to generalise previously known collective effects involving spins into new ones involving aggregates of harmonic oscillators or other degrees of freedom. It also explains how collective effects can be engineered to be robust against both disorder and noise, paving the way for more resilient quantum devices.

quant-ph↗

arXiv2025

Any type of spectroscopy can be efficiently simulated on a quantum computer

Spectroscopy is the most important method for probing the structure of molecules. However, predicting molecular spectra on classical computers is computationally expensive, with the most accurate methods having a cost that grows exponentially with molecule size. Quantum computers have been shown to simulate simple types of optical spectroscopy efficiently -- with a cost polynomial in molecule size -- using methods such as time-dependent simulations of photoinduced wavepackets. Here, we show that any type of spectroscopy can be efficiently simulated on a quantum computer using a time-domain approach, including spectroscopies of any order, any frequency range, and involving both electric and magnetic transitions. Our method works by computing any spectroscopic correlation function based on the corresponding double-sided Feynman diagram, the canonical description of spectroscopic interactions. The approach can be used to simulate spectroscopy of both closed and open molecular systems using both digital and analog quantum computers.

quant-ph↗

arXiv2025

Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics

Simulating the coupled electronic and nuclear response of a molecule to light excitation requires the application of nonadiabatic molecular dynamics. However, when faced with a specific photophysical or photochemical problem, selecting the most suitable theoretical approach from the wide array of available techniques is not a trivial task. The challenge is further complicated by the lack of systematic method comparisons and rigorous testing on realistic molecular systems. This absence of comprehensive molecular benchmarks remains a major obstacle to advances within the field of nonadiabatic molecular dynamics. A CECAM workshop, Standardizing Nonadiabatic Dynamics: Towards Common Benchmarks, was held in May 2024 to address this issue. This Perspective highlights the key challenges identified during the workshop in defining molecular benchmarks for nonadiabatic dynamics. Specifically, this work outlines some preliminary observations on essential components needed for simulations and proposes a roadmap aiming to establish, as an ultimate goal, a community-driven, standardized molecular benchmark set.

physics.chem-ph↗

arXiv2025

Engineering Quantum-Enhanced Transport by Supertransfer

Collective behaviour of the components of a quantum system can significantly alter the rates of dynamical processes within the system. A paradigmatic collective effect is superradiance, the enhancement in the rate that radiation is emitted by a group of emitters relative to that emitted by independent emitters. Less studied are collective effects in energy transport, notably supertransfer, the enhancement of the rate of energy transfer from donors to acceptors due to delocalised excitations. Despite its proposed significance in photosynthesis, there has been no direct experimental detection of supertransfer because, in biological or molecular systems, delocalisation cannot be turned on and off to evaluate its effect on energy transfer. Here, we show that supertransfer could be directly observed using a quantum device based on a superconducting circuit. The programmability and control offered by an engineered device would allow controllable delocalisation of quantum states, giving full tunability over supertransfer. Our guidelines for engineering supertransfer could inform the design of future quantum-enhanced light harvesters.

quant-ph↗

arXiv2023

Light-harvesting efficiency cannot depend on optical coherence in the absence of orientational order

The coherence of light has been proposed as a quantum-mechanical control for enhancing light-harvesting efficiency. In particular, optical coherence can be manipulated by changing either the polarization state or spectral phase of the light. Here, we show that, in weak light, light-harvesting efficiency cannot be controlled using any form of optical coherence in molecular light-harvesting systems and, more broadly, those comprising orientationally disordered sub-units and operating on longer-than-ultrafast timescales. Under those conditions, optical coherence does not affect light-harvesting efficiency, meaning that it cannot be used for control. Specifically, polarization-state control is lost in disordered samples or when the molecules reorient on the timescales of the light-harvesting, and spectral-phase control is lost when the efficiency is time-averaged for longer than the optical coherence time. In practice, efficiency is always averaged over long times, meaning that coherent optical control is only possible through polarisation in systems with orientational order.

physics.chem-ph↗

arXiv2023

Delocalisation enables efficient charge generation in organic photovoltaics, even with little to no energetic offset

Organic photovoltaics (OPVs) are promising candidates for solar-energy conversion, with device efficiencies continuing to increase. However, the precise mechanism of how charges separate in OPVs is not well understood because low dielectric constants produce a strong attraction between the charges, which they must overcome to separate. Separation has been thought to require energetic offsets at donor-acceptor interfaces, but recent materials have enabled efficient charge generation with small offsets, or with none at all in neat materials. Here, we extend delocalised kinetic Monte Carlo (dKMC) to develop a three-dimensional model of charge generation that includes disorder, delocalisation, and polaron formation in every step from photoexcitation to charge separation. Our simulations show that delocalisation dramatically increases charge-generation efficiency, partly by enabling excitons to dissociate in the bulk. Therefore, charge generation can be efficient even in devices with little to no energetic offset, including neat materials. Our findings demonstrate that the underlying quantum-mechanical effect that improves the charge-separation kinetics is faster and longer-distance hops between delocalised states, mediated by hybridised states of exciton and charge-transfer character.

cond-mat.mtrl-sci↗

arXiv2023

Fast and Accurate Simulations of Partially Delocalised Charge Separation in Organic Semiconductors

Accurate computational screening of candidate materials promises to accelerate the discovery of higher-efficiency organic photovoltaics (OPVs). However, modelling charge separation in OPVs is challenging because accurate models must include disorder, polaron formation, and charge delocalisation. Delocalised kinetic Monte Carlo (dKMC) includes these three essential ingredients, but it suffers from high computational cost. Recently, we developed jumping kinetic Monte Carlo (jKMC), a computationally cheap and accurate model of delocalised charge transport that models transport over a lattice of identical, spherical polarons. Here, we extend jKMC to describe the separation of a charge-transfer state, showing that this simplified approach can reproduce the considerable improvements in charge-separation efficiencies caused by delocalisation and first seen in dKMC. The low computational cost and simplicity of jKMC allows it to be applied to parameter regimes intractable by dKMC, and ensures jKMC can be easily incorporated into any existing KMC model.

physics.chem-ph↗

arXiv2023

Direct observation of geometric phase in dynamics around a conical intersection

Conical intersections are ubiquitous in chemistry and physics, often governing processes such as light harvesting, vision, photocatalysis, and chemical reactivity. They act as funnels between electronic states of molecules, allowing rapid and efficient relaxation during chemical dynamics. In addition, when a reaction path encircles a conical intersection, the molecular wavefunction experiences a geometric phase, which can affect the outcome of the reaction through quantum-mechanical interference. Past experiments have measured indirect signatures of geometric phases in scattering patterns and spectroscopic observables, but there has been no direct observation of the underlying wavepacket interference. Here, we experimentally observe geometric-phase interference in the dynamics of a wavepacket travelling around an engineered conical intersection in a programmable trapped-ion quantum simulator. To achieve this, we develop a technique to reconstruct the two-dimensional wavepacket densities of a trapped ion. Experiments agree with the theoretical model, demonstrating the ability of analog quantum simulators -- such as those realised using trapped ions -- to accurately describe nuclear quantum effects.

quant-ph↗

arXiv2023

Predicting molecular vibronic spectra using time-domain analog quantum simulation

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$_2$.

quant-ph↗

arXiv2022

Mechanism of delocalisation-enhanced exciton transport in disordered organic semiconductors

Large exciton diffusion lengths generally improve the performance of organic semiconductor devices, since they enable energy to be transported farther during the exciton lifetime. However, the physics of exciton motion in disordered organic materials is not fully understood, and modelling the transport of quantum-mechanically delocalised excitons in disordered organic semiconductors is a computational challenge. Here, we describe delocalised kinetic Monte Carlo (dKMC), the first model of three-dimensional exciton transport in organic semiconductors that includes delocalisation, disorder, and polaron formation. We find that delocalisation can dramatically increase exciton transport; for example, delocalisation across less than two molecules in each direction can increase the exciton diffusion coefficient by over an order of magnitude. The mechanism for the enhancement is twofold: delocalisation enables excitons both to hop more frequently and further in each hop. We also quantify the effect of transient delocalisation (short-lived periods where excitons become highly delocalised), and show it depends strongly on the disorder and the transition dipole moments.

physics.chem-ph↗

arXiv2022

Jumping kinetic Monte Carlo: Fast and accurate simulations of partially delocalised charge transport in organic semiconductors

Developing devices using disordered organic semiconductors requires accurate and practical models of charge transport. In these materials, charge transport occurs through partially delocalised states in an intermediate regime between localised hopping and delocalised band conduction. Partial delocalisation can increase mobilities by orders of magnitude over conventional hopping, making it important for materials and device design. Although delocalisation, disorder, and polaron formation can be described using delocalised kinetic Monte Carlo (dKMC), it is a computationally expensive method. Here, we develop jumping kinetic Monte Carlo (jKMC), a model that approaches the accuracy of dKMC with a computational cost comparable to conventional hopping. jKMC achieves its computational performance by modelling conduction using identical spherical polarons, yielding a simple delocalisation correction to the Marcus hopping rate that allows polarons to jump over their nearest neighbours. jKMC can be used in regimes of partial delocalisation inaccessible to dKMC to show that modest delocalisation can increase mobilities by as much as two orders of magnitude.

physics.chem-ph↗

arXiv2022

Even a little delocalization produces large kinetic enhancements of charge-separation efficiency in organic photovoltaics

In organic photovoltaics, charges can separate efficiently even if their Coulomb attraction is an order of magnitude greater than the available thermal energy. Delocalization has been suggested to explain this fact, because it could increase the initial separation of charges in the charge-transfer (CT) state, reducing their attraction. However, understanding the mechanism requires a kinetic model of delocalized charge separation, which has proven difficult because it involves tracking the correlated quantum-mechanical motion of the electron and the hole in large simulation boxes required for disordered materials. Here, we report the first three-dimensional simulations of charge-separation dynamics in the presence of disorder, delocalization, and polaron formation, finding that even slight delocalization, across less than two molecules, can substantially enhance the charge-separation efficiency, even starting with thermalized CT states. Delocalization does not enhance efficiency by reducing the Coulomb attraction; instead, the enhancement is a kinetic effect produced by the increased overlap of electronic states.

physics.chem-ph↗