Chiral-induced spin selectivity (CISS) enables spin selectivity of charge carriers in chiral molecular systems without magnetic materials. While spin selectivity has been widely investigated, its quantum coherence has not yet been explored. Here, we investigate spin-dependent photoluminescence (PL) dynamics in multilayer quantum-dot (QD) assemblies coupled by chiral linkers. Using circularly polarized excitation in the presence of an external magnetic field, we observe a pronounced modulation of the PL lifetime that depends on the magnetic field magnitude and geometry. The lifetime difference between left- and right-circularly polarized excitations exhibits a field-angle dependence, consistent with spin precession driven by the transverse magnetic-field component relative to the chiral axis. A model incorporating coupled spin precession and decay processes reproduces the experimental trends. These results establish chiral QD assemblies as a room-temperature platform for probing quantum coherent manifestations of the CISS effect, with implications for spintronic and quantum technologies.
Chiral-induced spin selectivity (CISS) enables spin selectivity of charge carriers in chiral molecular systems without magnetic materials. While spin selectivity has been widely investigated, its quantum coherence has not yet been explored. Here, we investigate spin-dependent photoluminescence (PL) dynamics in multilayer quantum-dot (QD) assemblies coupled by chiral linkers. Using circularly polarized excitation in the presence of an external magnetic field, we observe a pronounced modulation of the PL lifetime that depends on the magnetic field magnitude and geometry. The lifetime difference between left- and right-circularly polarized excitations exhibits a field-angle dependence, consistent with spin precession driven by the transverse magnetic-field component relative to the chiral axis. A model incorporating coupled spin precession and decay processes reproduces the experimental trends. These results establish chiral QD assemblies as a room-temperature platform for probing quantum coherent manifestations of the CISS effect, with implications for spintronic and quantum technologies.
The chirality-induced spin selectivity (CISS) effect has been invoked to explain recent reports of differences in the time-resolved EPR signals between chiral and achiral molecules. However, the microscopic origin of these differences and their connection to CISS remains contested, particularly since these systems lack a metal interface. Here we introduce an intramolecular spinterface-like mechanism that naturally arises within donor-chiral bridge-acceptor (D--χB--A) complexes and quantitatively reproduces experimentally reported observed spin polarization in time-resolved EPR studies. In our two-electron Lindblad model, the photoexcited charge-transfer electron traversing the chiral bridge exchanges with the residual donor electron, which acts as a localized magnetic moment analogous to an induced magnetic moment on an electrode surface. The resulting through-bridge charge current produces an effective solenoidal field at the donor--bridge interface, breaking spin degeneracy and directional symmetry, thus enabling spin-selective transport without invoking intrinsic spin-orbit coupling on the bridge. We show that the interplay between this current-induced field, donor thermalization (which breaks time-reversal symmetry), and bridge spin mixing yields tens-of-percent polarization over realistic experimental conditions and charge-transfer time scales, matching reported CISS signatures in triads and DNA hairpins. By explicitly resolving the dependence on solenoidal coupling strength, temperature, and spin-mixing rates, the model identifies the regime in which internal spinterfaces can generate robust CISS-like spin filtering. These findings demonstrate that CISS-like signals in isolated D--χB--A complexes are fully compatible with a spinterface mechanism, providing a unified conceptual framework for interpreting both device-based and molecule-internal CISS platforms.
Whether chirality-induced spin selectivity (CISS) reflects coherent SU(2) spin rotation or incoherent spin-dependent filtering is a central unresolved question in molecular spintronics, with implications ranging from asymmetric chemistry to quantum information. We show that these two scenarios are distinguishable by a sharp symmetry criterion on the superexchange interaction mediated by a chiral molecular bridge. Coherent CISS, implemented as a unitary spin rotation of the tunneling electron, generates a giant Dzyaloshinskii-Moriya (DM) interaction with ratio |D|/JH up to 3, which is two orders of magnitude beyond intrinsic Rashba spin-orbit coupling in Si/SiGe. Incoherent CISS, represented by any Hermitian (non-unitary but spin-diagonal) tunneling matrix, produces D = 0 identically; we prove this as a structural theorem, reinforced by a Lindblad argument that dissipative spin filtering cannot modify virtual-tunneling-mediated superexchange. The DM interaction thus serves as a coherence order parameter, nonzero only when quantum amplitudes for opposite-spin transmission maintain a fixed relative phase. We derive closed-form angular, enantiomeric, and sensitivity signatures and show that the critical coherent rotation angle lies two orders of magnitude below current transport-inferred values and is accessible to existing 10 kHz exchange spectroscopy in gate-defined quantum dots. Five candidate molecules are predicted to exceed this threshold by one to two orders of magnitude even in a conservative interface-amplification scenario. The proposed measurement converts a long-standing transport controversy into a binary spin-qubit experiment with quantum-amplitude resolution.
The optically-induced coherent spin dynamics in a charged quantum dot (QD) is studied theoretically using a new dynamical model for rigorous description of circularly polarized ultrashort optical pulse resonant interactions with the electron-trion system. Generalized pseudospin master equation is derived for description of the time evolution of spin coherences and spin populations in terms of the real state pseudospin (coherence) vector including dissipation in the system through spin relaxation processes. The equation is solved in the time domain self-consistently with the vector Maxwell equations for the optical wave propagation coupled to it via macroscopic medium polarization. Using the model the long-lived electron spin coherence left behind a single resonant ultrashort optical excitation of the electron-trion transition in a charged QD is simulated in the lowand high-intensity Rabi oscillations regime. Signatures of the polarized photoluminescence (PL) resulting from the numerical simulations, such as the appearance of a second echo pulse after the excitation and a characteristic PL trace shape, specific for initial spin-up orientation, are discussed for realization of high-fidelity schemes for coherent readout of a single spin polarization state.
Self-assembled quantum dots (QDs) containing a single electron are one of the leading candidate systems for the realization of a quantum computer. The spin states of charges confined in these dots have been shown to possess a number of qualities that are attractive for use as the quantum bits (qubits) in quantum computing implementations, particularly their long lifetimes and coherence times. In addition, these spin qubits may be controlled optically, offering the prospect of ultrafast qubit gate operations, a crucial necessity for the execution of quantum algorithms. Due to the weak interaction of self-assembled QDs with light, however, the coherent optical control and read-out of the spin states of charged self-assembled QDs has proven to be a considerable challenge. This thesis presents two sets of experiments demonstrating the coherent optical control and read-out of the quantum states of a self-assembled InAs QD containing a single electron. The first utilizes mode-locked picosecond optical pulses to control the optical transitions in the dot and to detect QD level occupations. These capabilities are used to observe transient phenomena in a singly charged InAs QD such as the generation and decay of excited state population and spin precession. Further, Rabi oscillations between the electron and the lowest-lying excited state are observed, demonstrating the ability to coherently control the optical transitions of the QD, a prerequisite for spin control. These results are built upon in the second set of experiments, in which a combination of optical pulses, an externally applied DC magnetic field and a continuous-wave (CW) optical field are employed to initialize and completely control the states of a QD confined electron spin. Spin control by the use of pulse-driven two-photon Raman processes, spin precession about the external magnetic field and geometric phases generated by CW-driven cyclic evolutions in the dot is demonstrated. A number of spin qubit gate operations are shown for these spin control mechanisms, forming a foundational set of single qubit gates required for the implementation of quantum computing with singly charged self-assembled QDs.
In photoluminescence kinetics of the InP quantum dots, we have found a long-lived component of the degree of circular polarization, showing practically no decay during the lifetime of excitation. It is shown that this effect is observed only in the charged quantum dots. The amplitude of the long-lived PL polarization can be controlled by an applied electric field and may be as high as 50% in the case of quasi resonance excitation. The existence of the long-lived component of the polarization is the clear evidence of large lifetime of the electron spin polarization in quantum dots.
The impact of hole g-factor anisotropy on spin-photon entanglement generation with InGaAs quantum dots
Self-assembled InGaAs/GaAs quantum dots (QDs) are of particular importance for the deterministic generation of spin-photon entanglement. One promising scheme relies on the Larmor precession of a spin in a transverse magnetic field, which is governed by the in-plane g-factors of the electron and valence band heavy-hole. We probe the origin of heavy-hole g-factor anisotropy with respect to the in-plane magnetic field direction and uncover how it impacts the entanglement generated between the spin and the photon polarization. First, using polarization-resolved photoluminescence measurements on a single QD, we determine that the impact of valence-band mixing dominates over effects due to a confinement-renormalized cubic Luttinger q parameter. From this, we construct a comprehensive hole g-tensor model. We then use this model to simulate the concurrence and fidelity of spin-photon entanglement generation with anisotropic hole g-factors, which can be tuned via magnetic field angle and excitation polarization. The results demonstrate that post-growth control of the hole g-factor can be used to improve spin-photon cluster state generation.